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

    <schemaVersion>X0306</schemaVersion>

    <documentType>4</documentType>

    <periodOfReport>2021-06-28</periodOfReport>

    <issuer>
        <issuerCik>0000748592</issuerCik>
        <issuerName>Brooklyn ImmunoTherapeutics, Inc.</issuerName>
        <issuerTradingSymbol>BTX</issuerTradingSymbol>
    </issuer>

    <reportingOwner>
        <reportingOwnerId>
            <rptOwnerCik>0001870486</rptOwnerCik>
            <rptOwnerName>DAmour Kevin</rptOwnerName>
        </reportingOwnerId>
        <reportingOwnerAddress>
            <rptOwnerStreet1>C/O BROOKLYN IMMUNOTHERAPEUTICS, INC.</rptOwnerStreet1>
            <rptOwnerStreet2>140 58TH STREET, BUILDING A, SUITE 2100</rptOwnerStreet2>
            <rptOwnerCity>BROOKLYN</rptOwnerCity>
            <rptOwnerState>NY</rptOwnerState>
            <rptOwnerZipCode>11220</rptOwnerZipCode>
            <rptOwnerStateDescription></rptOwnerStateDescription>
        </reportingOwnerAddress>
        <reportingOwnerRelationship>
            <isOfficer>true</isOfficer>
            <officerTitle>See Remarks</officerTitle>
        </reportingOwnerRelationship>
    </reportingOwner>

    <derivativeTable>
        <derivativeTransaction>
            <securityTitle>
                <value>Stock Option</value>
            </securityTitle>
            <conversionOrExercisePrice>
                <value>21.35</value>
            </conversionOrExercisePrice>
            <transactionDate>
                <value>2021-06-28</value>
            </transactionDate>
            <transactionCoding>
                <transactionFormType>4</transactionFormType>
                <transactionCode>A</transactionCode>
                <equitySwapInvolved>0</equitySwapInvolved>
            </transactionCoding>
            <transactionAmounts>
                <transactionShares>
                    <value>140580</value>
                </transactionShares>
                <transactionPricePerShare>
                    <value>0</value>
                </transactionPricePerShare>
                <transactionAcquiredDisposedCode>
                    <value>A</value>
                </transactionAcquiredDisposedCode>
            </transactionAmounts>
            <exerciseDate>
                <footnoteId id="F1"/>
            </exerciseDate>
            <expirationDate>
                <value>2031-06-28</value>
            </expirationDate>
            <underlyingSecurity>
                <underlyingSecurityTitle>
                    <value>Common Stock</value>
                </underlyingSecurityTitle>
                <underlyingSecurityShares>
                    <value>140580</value>
                </underlyingSecurityShares>
            </underlyingSecurity>
            <postTransactionAmounts>
                <sharesOwnedFollowingTransaction>
                    <value>140580</value>
                </sharesOwnedFollowingTransaction>
            </postTransactionAmounts>
            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>D</value>
                </directOrIndirectOwnership>
            </ownershipNature>
        </derivativeTransaction>
        <derivativeTransaction>
            <securityTitle>
                <value>Restricted Stock Unit</value>
            </securityTitle>
            <conversionOrExercisePrice>
                <footnoteId id="F2"/>
            </conversionOrExercisePrice>
            <transactionDate>
                <value>2021-06-28</value>
            </transactionDate>
            <transactionCoding>
                <transactionFormType>4</transactionFormType>
                <transactionCode>A</transactionCode>
                <equitySwapInvolved>0</equitySwapInvolved>
            </transactionCoding>
            <transactionAmounts>
                <transactionShares>
                    <value>70290</value>
                </transactionShares>
                <transactionPricePerShare>
                    <value>0</value>
                </transactionPricePerShare>
                <transactionAcquiredDisposedCode>
                    <value>A</value>
                </transactionAcquiredDisposedCode>
            </transactionAmounts>
            <exerciseDate>
                <footnoteId id="F3"/>
            </exerciseDate>
            <expirationDate>
                <value>2031-06-28</value>
            </expirationDate>
            <underlyingSecurity>
                <underlyingSecurityTitle>
                    <value>Common Stock</value>
                </underlyingSecurityTitle>
                <underlyingSecurityShares>
                    <value>70290</value>
                </underlyingSecurityShares>
            </underlyingSecurity>
            <postTransactionAmounts>
                <sharesOwnedFollowingTransaction>
                    <value>70290</value>
                </sharesOwnedFollowingTransaction>
            </postTransactionAmounts>
            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>D</value>
                </directOrIndirectOwnership>
            </ownershipNature>
        </derivativeTransaction>
    </derivativeTable>

    <footnotes>
        <footnote id="F1">The option vests and becomes exercisable over four years, with twenty-five percent of the shares covered thereby vesting on June 28, 2022, and 1/36 of the remaining shares covered thereby vesting on the 28th day of each calendar month from July 28, 2022 through June 28, 2025, subject to continued service through each vesting date.</footnote>
        <footnote id="F2">Each restricted stock unit represents a contingent right to receive one share of common stock.</footnote>
        <footnote id="F3">The Restricted Stock Unit vests and becomes exercisable in four equal installments on June 28 of each of 2022, 2023, 2024 and 2025, provided they shall vest in full immediately prior to a Change in Control (as defined in Dr. D'Amour's Executive Employment Agreement, dated as of June 5, 2021 and effective as of June 28, 2021), subject to continued service through each vesting date.</footnote>
    </footnotes>

    <remarks>Chief Scientific Officer</remarks>

    <ownerSignature>
        <signatureName>/s/Bella Zaslavsky, Attorney-in-Fact for Kevin D'Amour</signatureName>
        <signatureDate>2021-06-30</signatureDate>
    </ownerSignature>
</ownershipDocument>
