<?xml version="1.0"?>
<ownershipDocument>

    <schemaVersion>X0303</schemaVersion>

    <documentType>4</documentType>

    <periodOfReport>2011-03-03</periodOfReport>

    <notSubjectToSection16>0</notSubjectToSection16>

    <issuer>
        <issuerCik>0001501364</issuerCik>
        <issuerName>Rockville Financial, Inc. /CT/</issuerName>
        <issuerTradingSymbol>RCKBD</issuerTradingSymbol>
    </issuer>

    <reportingOwner>
        <reportingOwnerId>
            <rptOwnerCik>0001410571</rptOwnerCik>
            <rptOwnerName>Kucia Mark A</rptOwnerName>
        </reportingOwnerId>
        <reportingOwnerAddress>
            <rptOwnerStreet1>ROCKVILLE FINANCIAL NEW, INC.</rptOwnerStreet1>
            <rptOwnerStreet2>1645  ELLINGTON ROAD</rptOwnerStreet2>
            <rptOwnerCity>SOUTH WINDSOR</rptOwnerCity>
            <rptOwnerState>CT</rptOwnerState>
            <rptOwnerZipCode>06074</rptOwnerZipCode>
            <rptOwnerStateDescription></rptOwnerStateDescription>
        </reportingOwnerAddress>
        <reportingOwnerRelationship>
            <isDirector>0</isDirector>
            <isOfficer>0</isOfficer>
            <isTenPercentOwner>0</isTenPercentOwner>
            <isOther>1</isOther>
            <officerTitle></officerTitle>
            <otherText>SVP, Rockville Bank</otherText>
        </reportingOwnerRelationship>
    </reportingOwner>

    <nonDerivativeTable>
        <nonDerivativeTransaction>
            <securityTitle>
                <value>Common Stock</value>
            </securityTitle>
            <transactionDate>
                <value>2011-03-03</value>
            </transactionDate>
            <deemedExecutionDate></deemedExecutionDate>
            <transactionCoding>
                <transactionFormType>4</transactionFormType>
                <transactionCode>J</transactionCode>
                <equitySwapInvolved>0</equitySwapInvolved>
            </transactionCoding>
            <transactionAmounts>
                <transactionShares>
                    <value>4204</value>
                </transactionShares>
                <transactionPricePerShare>
                    <value>0.00</value>
                    <footnoteId id="F1"/>
                </transactionPricePerShare>
                <transactionAcquiredDisposedCode>
                    <value>A</value>
                </transactionAcquiredDisposedCode>
            </transactionAmounts>
            <postTransactionAmounts>
                <sharesOwnedFollowingTransaction>
                    <value>4204</value>
                </sharesOwnedFollowingTransaction>
            </postTransactionAmounts>
            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>I</value>
                </directOrIndirectOwnership>
                <natureOfOwnership>
                    <value>By Rockville Bank 401(k) Plan</value>
                </natureOfOwnership>
            </ownershipNature>
        </nonDerivativeTransaction>
        <nonDerivativeTransaction>
            <securityTitle>
                <value>Common Stock</value>
                <footnoteId id="F2"/>
            </securityTitle>
            <transactionDate>
                <value>2011-03-03</value>
            </transactionDate>
            <deemedExecutionDate></deemedExecutionDate>
            <transactionCoding>
                <transactionFormType>4</transactionFormType>
                <transactionCode>J</transactionCode>
                <equitySwapInvolved>0</equitySwapInvolved>
            </transactionCoding>
            <transactionAmounts>
                <transactionShares>
                    <value>9277</value>
                </transactionShares>
                <transactionPricePerShare>
                    <value>0.00</value>
                    <footnoteId id="F1"/>
                </transactionPricePerShare>
                <transactionAcquiredDisposedCode>
                    <value>A</value>
                </transactionAcquiredDisposedCode>
            </transactionAmounts>
            <postTransactionAmounts>
                <sharesOwnedFollowingTransaction>
                    <value>9277</value>
                </sharesOwnedFollowingTransaction>
            </postTransactionAmounts>
            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>I</value>
                </directOrIndirectOwnership>
                <natureOfOwnership>
                    <value>By Rockville Bank ESOP Plan</value>
                </natureOfOwnership>
            </ownershipNature>
        </nonDerivativeTransaction>
        <nonDerivativeTransaction>
            <securityTitle>
                <value>Common Stock</value>
                <footnoteId id="F3"/>
                <footnoteId id="F4"/>
                <footnoteId id="F5"/>
            </securityTitle>
            <transactionDate>
                <value>2011-03-03</value>
            </transactionDate>
            <deemedExecutionDate></deemedExecutionDate>
            <transactionCoding>
                <transactionFormType>4</transactionFormType>
                <transactionCode>J</transactionCode>
                <equitySwapInvolved>0</equitySwapInvolved>
            </transactionCoding>
            <transactionAmounts>
                <transactionShares>
                    <value>9717</value>
                </transactionShares>
                <transactionPricePerShare>
                    <value>0.00</value>
                    <footnoteId id="F1"/>
                </transactionPricePerShare>
                <transactionAcquiredDisposedCode>
                    <value>A</value>
                </transactionAcquiredDisposedCode>
            </transactionAmounts>
            <postTransactionAmounts>
                <sharesOwnedFollowingTransaction>
                    <value>9717</value>
                </sharesOwnedFollowingTransaction>
            </postTransactionAmounts>
            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>D</value>
                </directOrIndirectOwnership>
            </ownershipNature>
        </nonDerivativeTransaction>
    </nonDerivativeTable>

    <derivativeTable>
        <derivativeTransaction>
            <securityTitle>
                <value>Stock Options</value>
                <footnoteId id="F6"/>
                <footnoteId id="F7"/>
            </securityTitle>
            <conversionOrExercisePrice>
                <value>7.90</value>
            </conversionOrExercisePrice>
            <transactionDate>
                <value>2011-03-03</value>
            </transactionDate>
            <deemedExecutionDate></deemedExecutionDate>
            <transactionCoding>
                <transactionFormType>4</transactionFormType>
                <transactionCode>J</transactionCode>
                <equitySwapInvolved>0</equitySwapInvolved>
            </transactionCoding>
            <transactionAmounts>
                <transactionShares>
                    <value>9858</value>
                </transactionShares>
                <transactionPricePerShare>
                    <value>0.00</value>
                </transactionPricePerShare>
                <transactionAcquiredDisposedCode>
                    <value>A</value>
                </transactionAcquiredDisposedCode>
            </transactionAmounts>
            <exerciseDate>
                <value>2008-02-20</value>
            </exerciseDate>
            <expirationDate>
                <value>2018-02-20</value>
            </expirationDate>
            <underlyingSecurity>
                <underlyingSecurityTitle>
                    <value>Common Stock</value>
                </underlyingSecurityTitle>
                <underlyingSecurityShares>
                    <value>9858</value>
                </underlyingSecurityShares>
            </underlyingSecurity>
            <postTransactionAmounts>
                <sharesOwnedFollowingTransaction>
                    <value>9858</value>
                </sharesOwnedFollowingTransaction>
            </postTransactionAmounts>
            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>D</value>
                </directOrIndirectOwnership>
            </ownershipNature>
        </derivativeTransaction>
        <derivativeTransaction>
            <securityTitle>
                <value>Stock Options</value>
                <footnoteId id="F6"/>
                <footnoteId id="F8"/>
            </securityTitle>
            <conversionOrExercisePrice>
                <value>6.09</value>
            </conversionOrExercisePrice>
            <transactionDate>
                <value>2011-03-03</value>
            </transactionDate>
            <deemedExecutionDate></deemedExecutionDate>
            <transactionCoding>
                <transactionFormType>4</transactionFormType>
                <transactionCode>J</transactionCode>
                <equitySwapInvolved>0</equitySwapInvolved>
            </transactionCoding>
            <transactionAmounts>
                <transactionShares>
                    <value>9479</value>
                </transactionShares>
                <transactionPricePerShare>
                    <value>0.00</value>
                </transactionPricePerShare>
                <transactionAcquiredDisposedCode>
                    <value>A</value>
                </transactionAcquiredDisposedCode>
            </transactionAmounts>
            <exerciseDate>
                <value>2009-03-16</value>
            </exerciseDate>
            <expirationDate>
                <value>2019-03-16</value>
            </expirationDate>
            <underlyingSecurity>
                <underlyingSecurityTitle>
                    <value>Common Stock</value>
                </underlyingSecurityTitle>
                <underlyingSecurityShares>
                    <value>9479</value>
                </underlyingSecurityShares>
            </underlyingSecurity>
            <postTransactionAmounts>
                <sharesOwnedFollowingTransaction>
                    <value>9479</value>
                </sharesOwnedFollowingTransaction>
            </postTransactionAmounts>
            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>D</value>
                </directOrIndirectOwnership>
            </ownershipNature>
        </derivativeTransaction>
        <derivativeTransaction>
            <securityTitle>
                <value>Stock Options</value>
                <footnoteId id="F6"/>
                <footnoteId id="F9"/>
            </securityTitle>
            <conversionOrExercisePrice>
                <value>7.42</value>
            </conversionOrExercisePrice>
            <transactionDate>
                <value>2011-03-03</value>
            </transactionDate>
            <deemedExecutionDate></deemedExecutionDate>
            <transactionCoding>
                <transactionFormType>4</transactionFormType>
                <transactionCode>J</transactionCode>
                <equitySwapInvolved>0</equitySwapInvolved>
            </transactionCoding>
            <transactionAmounts>
                <transactionShares>
                    <value>5187</value>
                </transactionShares>
                <transactionPricePerShare>
                    <value>0.00</value>
                </transactionPricePerShare>
                <transactionAcquiredDisposedCode>
                    <value>A</value>
                </transactionAcquiredDisposedCode>
            </transactionAmounts>
            <exerciseDate>
                <value>2010-11-15</value>
            </exerciseDate>
            <expirationDate>
                <value>2020-11-15</value>
            </expirationDate>
            <underlyingSecurity>
                <underlyingSecurityTitle>
                    <value>Common Stock</value>
                </underlyingSecurityTitle>
                <underlyingSecurityShares>
                    <value>5187</value>
                </underlyingSecurityShares>
            </underlyingSecurity>
            <postTransactionAmounts>
                <sharesOwnedFollowingTransaction>
                    <value>5187</value>
                </sharesOwnedFollowingTransaction>
            </postTransactionAmounts>
            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>D</value>
                </directOrIndirectOwnership>
            </ownershipNature>
        </derivativeTransaction>
    </derivativeTable>

    <footnotes>
        <footnote id="F1">Pursuant to the Plan of Conversion and Reorganization, each share of Rockville Financial, Inc. was exchanged for 1.5167 shares of Rockville Financial New, Inc.</footnote>
        <footnote id="F2">Shares allocated to the account of Mr. Kucia under the Rockville Bank Employee Stock Ownership Plan, of which 7419.200 shares are vested as of March 3, 2011.</footnote>
        <footnote id="F3">Includes 4,264 shares of restricted stock granted pursuant to the Rockville Financial, Inc. 2006 Stock Incentive Award Plan. The original grant of 4,000 shares (x 1.5167 exchange ratio becomes 6,066 shares) will become exercisable in equal 20% increments over a five year period, the first 20% becoming exercisable on February 20, 2008 and the subsequent vesting on each annual anniversary of that date. The reported number of shares is net of 1,188 shares (x 1.5167 exchange ratio becomes 1,801 shares) withheld by the Issuer for tax withholding purposes.</footnote>
        <footnote id="F4">Includes 2,575 restricted stock granted pursuant to the Rockville Financial, Inc. 2006 Stock Incentive Award Plan. The original grant of 2,000 shares (x 1.5167 exchange ratio becomes 3,033 shares) will become vested in equal 20% increments over a five year period, the first 20% vesting on March 16, 2009 and the subsequent vesting on each annual anniversary of that date. The reported number of shares is net of 302 shares (x 1.5167 exchange ratio becomes 458 shares) withheld by the Issuer for tax withholding purposes.</footnote>
        <footnote id="F5">Includes 2,740 restricted shares granted pursuant to the Rockville Financial, Inc. 2006 Stock Incentive Award Plan. The original grant of 2,000 shares (x 1.5167 exchange ratio becomes 3,033 shares) vest in equal 20% increments over a five year period, the first 20% vesting on November 15, 2010 and the subsequent vesting on each annual anniversary of that date. The reported number of shares is net of 103 shares (x 1.5167 exchange ratio becomes 156 shares) withheld by the Issuer for tax withholding purposes.</footnote>
        <footnote id="F6">Pursuant to the Plan of Conversion and Reorganization, each option to purchase a share of Rockville Financial, Inc. was converted into an option to purchase 1.5167 shares of Rockville Financial New, Inc. common stock, truncated down to the nearest whole share.  The exercise price per share for each converted option is determined by dividing the exercise price of such converted option by the 1.5167 exchange ratio, with such quotient rounded to the nearest whole cent.  All such options continue to vest according to their original terms.</footnote>
        <footnote id="F7">Stock options granted pursuant to the Rockville Financial, Inc. 2006 Stock Incentive Award Plan and will become exercisable in equal 20% increments over a five year period, the first 20% becoming exercisable on February 20, 2008 and the subsequent vesting on each annual anniversary of that date.</footnote>
        <footnote id="F8">Stock options granted pursuant to the Rockville Financial, Inc. 2006 Stock Incentive Award Plan and will become exercisable in equal 20% increments over a five year period, the first 20% becoming exercisable on March 16, 2009 and the subsequent vesting on each annual anniversary of that date.</footnote>
        <footnote id="F9">Stock options granted pursuant to the Rockville Financial, Inc. 2006 Stock Incentive Award Plan and will become exercisable in equal 20% increments over a five year period, the first 20% becoming exercisable on November 15, 2010 and the subsequent vesting on each annual anniversary of that date.</footnote>
    </footnotes>

    <remarks></remarks>

    <ownerSignature>
        <signatureName>/s/ Marliese L. Shaw by POA</signatureName>
        <signatureDate>2011-03-07</signatureDate>
    </ownerSignature>
</ownershipDocument>
