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

    <schemaVersion>X0206</schemaVersion>

    <documentType>3</documentType>

    <periodOfReport>2024-01-01</periodOfReport>

    <noSecuritiesOwned>0</noSecuritiesOwned>

    <issuer>
        <issuerCik>0001735948</issuerCik>
        <issuerName>Greenbrook TMS Inc.</issuerName>
        <issuerTradingSymbol>GBNH</issuerTradingSymbol>
    </issuer>

    <reportingOwner>
        <reportingOwnerId>
            <rptOwnerCik>0002005018</rptOwnerCik>
            <rptOwnerName>Burke Brian P</rptOwnerName>
        </reportingOwnerId>
        <reportingOwnerAddress>
            <rptOwnerStreet1>C/O GREENBROOK TMS. 890 YONGE STREET</rptOwnerStreet1>
            <rptOwnerStreet2>7TH FLOOR</rptOwnerStreet2>
            <rptOwnerCity>TORONTO</rptOwnerCity>
            <rptOwnerState>A6</rptOwnerState>
            <rptOwnerZipCode>M4W3P4</rptOwnerZipCode>
            <rptOwnerStateDescription>ONTARIO, CANADA</rptOwnerStateDescription>
        </reportingOwnerAddress>
        <reportingOwnerRelationship>
            <isDirector>1</isDirector>
            <isOfficer>0</isOfficer>
            <isTenPercentOwner>0</isTenPercentOwner>
            <isOther>0</isOther>
        </reportingOwnerRelationship>
    </reportingOwner>

    <derivativeTable>
        <derivativeHolding>
            <securityTitle>
                <value>Options</value>
            </securityTitle>
            <conversionOrExercisePrice>
                <value>10.00</value>
            </conversionOrExercisePrice>
            <exerciseDate>
                <footnoteId id="F1"/>
            </exerciseDate>
            <expirationDate>
                <value>2028-10-03</value>
            </expirationDate>
            <underlyingSecurity>
                <underlyingSecurityTitle>
                    <value>Common Shares</value>
                </underlyingSecurityTitle>
                <underlyingSecurityShares>
                    <value>6000</value>
                </underlyingSecurityShares>
            </underlyingSecurity>
            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>D</value>
                </directOrIndirectOwnership>
            </ownershipNature>
        </derivativeHolding>
        <derivativeHolding>
            <securityTitle>
                <value>Options</value>
            </securityTitle>
            <conversionOrExercisePrice>
                <value>10.13</value>
                <footnoteId id="F3"/>
            </conversionOrExercisePrice>
            <exerciseDate>
                <footnoteId id="F2"/>
            </exerciseDate>
            <expirationDate>
                <value>2030-02-03</value>
            </expirationDate>
            <underlyingSecurity>
                <underlyingSecurityTitle>
                    <value>Common Shares</value>
                </underlyingSecurityTitle>
                <underlyingSecurityShares>
                    <value>6000</value>
                </underlyingSecurityShares>
            </underlyingSecurity>
            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>D</value>
                </directOrIndirectOwnership>
            </ownershipNature>
        </derivativeHolding>
        <derivativeHolding>
            <securityTitle>
                <value>Deferred Share Units</value>
            </securityTitle>
            <conversionOrExercisePrice>
                <value>0.00</value>
                <footnoteId id="F4"/>
            </conversionOrExercisePrice>
            <exerciseDate>
                <footnoteId id="F4"/>
            </exerciseDate>
            <expirationDate>
                <footnoteId id="F5"/>
            </expirationDate>
            <underlyingSecurity>
                <underlyingSecurityTitle>
                    <value>Common Shares</value>
                </underlyingSecurityTitle>
                <underlyingSecurityShares>
                    <value>251018</value>
                    <footnoteId id="F6"/>
                </underlyingSecurityShares>
            </underlyingSecurity>
            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>D</value>
                </directOrIndirectOwnership>
            </ownershipNature>
        </derivativeHolding>
    </derivativeTable>

    <footnotes>
        <footnote id="F1">These options were granted pursuant to the Company's Amended Employee Stock Option Plan (the &quot;Stock Option Plan&quot;), as described in the Company's 2022 Meeting Information Circular, filed with the Securities and Exchange Commission on May 23, 2023. The options were granted on October 3, 2018 and fully vested on March 31, 2019 and accordingly, are all exercisable.</footnote>
        <footnote id="F2">These options were granted pursuant to the Stock Option Plan on February 3, 2020 and vested over a three year period, with one-third vesting on each of the 3 anniversaries of the date of the grant. As of the date hereof, all options are vested and exercisable.</footnote>
        <footnote id="F3">Converted to USD based on the average daily exchange rate of the Bank of Canada reported on December 29, 2023. Each option may be exercised for a price of $13.40 Canadian dollars.</footnote>
        <footnote id="F4">These deferred share units (&quot;DSUs&quot;) were granted between June 15, 2021 and December 15, 2023 pursuant to the DSU Plan for non-employee directors, as described in the Company's 2022 Meeting Information Circular, filed with the Securities and Exchange Commission on May 23, 2023. The DSUs immediately vest upon grant, but holders thereof are not entitled to receive a payment in respect of the value of their DSUs until their tenure on the board of directors ceases.</footnote>
        <footnote id="F5">The DSUs do not expire.</footnote>
        <footnote id="F6">Mr. Burke will receive a payment in cash at the fair market value of the common shares represented by his or her DSUs generally within ten days of his elected redemption date. Mr. Burke's elected redemption date will not be earlier than the date he ceases to hold all positions with the Company and will not be later than December 31 of the year following the year in which he ceases to hold all positions with the Company.</footnote>
    </footnotes>

    <remarks></remarks>

    <ownerSignature>
        <signatureName>/s/William Leonard, Attorney-in-Fact</signatureName>
        <signatureDate>2024-01-02</signatureDate>
    </ownerSignature>
</ownershipDocument>
