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It pretty easy to connect an O365 group to an existing SharePoint site collection through settings => Connect to new Office 365 Group.

But how can we connect an existing site collection to an existing O365 Group? Powershell is preferred but I would be interested to know if this is possible through the browser.

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As far as I know, it's not supported to connect an existing site collection to an existing O365 Group currently. You have to create a new group regardless of through powershell or UI.

Connect to an Office 365 group:https://docs.microsoft.com/en-us/sharepoint/dev/transform/modernize-connect-to-office365-group

Connect sites to new Office 365 groups using PowerShell: Set-SPOSiteOffice365Group

Connect sites to new Office 365 groups using the CSOM API:https://docs.microsoft.com/en-us/sharepoint/dev/features/groupify/groupify-csom

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