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

    <schemaVersion>X0206</schemaVersion>

    <documentType>3</documentType>

    <periodOfReport>2021-10-21</periodOfReport>

    <noSecuritiesOwned>0</noSecuritiesOwned>

    <issuer>
        <issuerCik>0001840233</issuerCik>
        <issuerName>Xilio Therapeutics, Inc.</issuerName>
        <issuerTradingSymbol>XLO</issuerTradingSymbol>
    </issuer>

    <reportingOwner>
        <reportingOwnerId>
            <rptOwnerCik>0001780602</rptOwnerCik>
            <rptOwnerName>SV7 Impact Medicine Fund LP</rptOwnerName>
        </reportingOwnerId>
        <reportingOwnerAddress>
            <rptOwnerStreet1>71 KINGSWAY</rptOwnerStreet1>
            <rptOwnerStreet2></rptOwnerStreet2>
            <rptOwnerCity>LONDON</rptOwnerCity>
            <rptOwnerState>X0</rptOwnerState>
            <rptOwnerZipCode>WC2B 6ST</rptOwnerZipCode>
            <rptOwnerStateDescription>UNITED KINGDOM</rptOwnerStateDescription>
        </reportingOwnerAddress>
        <reportingOwnerRelationship>
            <isDirector>0</isDirector>
            <isOfficer>0</isOfficer>
            <isTenPercentOwner>1</isTenPercentOwner>
            <isOther>0</isOther>
        </reportingOwnerRelationship>
    </reportingOwner>

    <reportingOwner>
        <reportingOwnerId>
            <rptOwnerCik>0001889859</rptOwnerCik>
            <rptOwnerName>SV7 (IMF) GP LLP</rptOwnerName>
        </reportingOwnerId>
        <reportingOwnerAddress>
            <rptOwnerStreet1>71 KINGSWAY</rptOwnerStreet1>
            <rptOwnerStreet2></rptOwnerStreet2>
            <rptOwnerCity>LONDON</rptOwnerCity>
            <rptOwnerState>X0</rptOwnerState>
            <rptOwnerZipCode>WC2B 6ST</rptOwnerZipCode>
            <rptOwnerStateDescription>UNITED KINGDOM</rptOwnerStateDescription>
        </reportingOwnerAddress>
        <reportingOwnerRelationship>
            <isDirector>0</isDirector>
            <isOfficer>0</isOfficer>
            <isTenPercentOwner>1</isTenPercentOwner>
            <isOther>0</isOther>
        </reportingOwnerRelationship>
    </reportingOwner>

    <derivativeTable>
        <derivativeHolding>
            <securityTitle>
                <value>Series B Convertible Preferred Stock</value>
            </securityTitle>
            <conversionOrExercisePrice>
                <value>0.00</value>
            </conversionOrExercisePrice>
            <exerciseDate>
                <footnoteId id="F1"/>
            </exerciseDate>
            <expirationDate>
                <footnoteId id="F1"/>
            </expirationDate>
            <underlyingSecurity>
                <underlyingSecurityTitle>
                    <value>Common Stock</value>
                    <footnoteId id="F1"/>
                </underlyingSecurityTitle>
                <underlyingSecurityShares>
                    <value>998544</value>
                </underlyingSecurityShares>
            </underlyingSecurity>
            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>D</value>
                </directOrIndirectOwnership>
            </ownershipNature>
        </derivativeHolding>
        <derivativeHolding>
            <securityTitle>
                <value>Series B Convertible Preferred Stock</value>
            </securityTitle>
            <conversionOrExercisePrice>
                <value>0.00</value>
            </conversionOrExercisePrice>
            <exerciseDate>
                <footnoteId id="F1"/>
            </exerciseDate>
            <expirationDate>
                <footnoteId id="F1"/>
            </expirationDate>
            <underlyingSecurity>
                <underlyingSecurityTitle>
                    <value>Common Stock</value>
                    <footnoteId id="F1"/>
                </underlyingSecurityTitle>
                <underlyingSecurityShares>
                    <value>998544</value>
                </underlyingSecurityShares>
            </underlyingSecurity>
            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>I</value>
                </directOrIndirectOwnership>
                <natureOfOwnership>
                    <value>See footnote</value>
                    <footnoteId id="F2"/>
                </natureOfOwnership>
            </ownershipNature>
        </derivativeHolding>
        <derivativeHolding>
            <securityTitle>
                <value>Series C Convertible Preferred Stock</value>
            </securityTitle>
            <conversionOrExercisePrice>
                <value>0.00</value>
            </conversionOrExercisePrice>
            <exerciseDate>
                <footnoteId id="F1"/>
            </exerciseDate>
            <expirationDate>
                <footnoteId id="F1"/>
            </expirationDate>
            <underlyingSecurity>
                <underlyingSecurityTitle>
                    <value>Common Stock</value>
                    <footnoteId id="F1"/>
                </underlyingSecurityTitle>
                <underlyingSecurityShares>
                    <value>302588</value>
                </underlyingSecurityShares>
            </underlyingSecurity>
            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>D</value>
                </directOrIndirectOwnership>
            </ownershipNature>
        </derivativeHolding>
        <derivativeHolding>
            <securityTitle>
                <value>Series C Convertible Preferred Stock</value>
            </securityTitle>
            <conversionOrExercisePrice>
                <value>0.00</value>
            </conversionOrExercisePrice>
            <exerciseDate>
                <footnoteId id="F1"/>
            </exerciseDate>
            <expirationDate>
                <footnoteId id="F1"/>
            </expirationDate>
            <underlyingSecurity>
                <underlyingSecurityTitle>
                    <value>Common Stock</value>
                    <footnoteId id="F1"/>
                </underlyingSecurityTitle>
                <underlyingSecurityShares>
                    <value>302588</value>
                </underlyingSecurityShares>
            </underlyingSecurity>
            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>I</value>
                </directOrIndirectOwnership>
                <natureOfOwnership>
                    <value>See footnote</value>
                    <footnoteId id="F2"/>
                </natureOfOwnership>
            </ownershipNature>
        </derivativeHolding>
    </derivativeTable>

    <footnotes>
        <footnote id="F1">Each share of Series B Convertible Preferred Stock and Series C Convertible Preferred Stock (together, the &quot;Preferred Stock&quot;) will automatically convert into 0.1053 shares of the Issuer's Common Stock immediately prior to the closing of the Issuer's initial public offering (the &quot;IPO&quot;). The Preferred Stock has no expiration date.</footnote>
        <footnote id="F2">Consists of shares of common stock underlying shares of convertible preferred stock held by SV7 Impact Medicine Fund LP, via its general partner SV7 (IMF) GP LLP. Catherine Bingham, Michael Ross, who is a member of our board of directors, and Houman Ashrafian are members of the investment committee of SV7 (IMF) GP LLP, which has voting and investment power with respect to these shares, and may be deemed to beneficially own such shares. SV7 (IMF) GP LLP and Ms. Bingham, Mr. Ross and Mr. Ashrafian each disclaim beneficial ownership of the shares held herein except to the extent of their pecuniary interest therein. The address of SV7 Impact Medicine Fund LP is 71 Kingsway, London, WC2B 6ST, United Kingdom.</footnote>
    </footnotes>

    <remarks>Exhibit 24.1: Power of Attorney (SV7 Impact Medicine Fund LP)
Exhibit 24.2: Power of Attorney (SV7 (IMF) GP LLP)</remarks>

    <ownerSignature>
        <signatureName>/s/ Kathleen R. Henry, pursuant to Power of Attorney for SV7 Impact Medicine Fund LP</signatureName>
        <signatureDate>2021-10-21</signatureDate>
    </ownerSignature>

    <ownerSignature>
        <signatureName>/s/ Kathleen R. Henry, pursuant to Power of Attorney for SV7 (IMF) GP LLP</signatureName>
        <signatureDate>2021-10-21</signatureDate>
    </ownerSignature>
</ownershipDocument>
