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I believe it defaults to the account you sign into first, so you can log out of all of your gmail accounts, and log into what your want your "default" to be first.

If you're using chrome and logged into your google account on chrome, I think you're already logged in.

I don't know how you'd do this if you didn't want your chrome account to be your "default" account. I personal use firefox.

FYI, Containers in Firefox make life much better for having multiple Google accounts signed in at the same time.

I thought I was doing something wrong! It NEVER defaults to the one I am expecting.