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This turned out to be super easy, but I couldn’t find it explained anywhere. If anyone knows where it is already documented, please link.
I had only one available “From Email” in my WP Mail SMTP settings screen. I had a bunch of other aliases set up for this Gsuite user. To add any or all of those users to that “From Email” dropdown list, you need to log into Gmail.com as the main Gsuite user, go to Settings / Accounts and add any alias you want to use as “From” mail on the web site to “Send Mail As”.
It appears in the dropdown list right away. This was so much easier than I thought it would be.