I would like to unlink this account from my XBL gamertag and link it to my PSN account. I do not want to use an entirely new account. Is this possible?
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Specifically, go to your Settings page, and click on "Account Settings". You will find buttons for the various types of accounts you can link to your profile (and unlink your existing ones). Note that you must have at least one account linked to your profile, and you cannot remove the one you are currently using to sign into bungie.net.