As someone who watches a lot of anime, I just thought she was doing that "The one loyal friend who will always believe in you turns around and smiles at you when you part ways to assure the audience that they're a loyal friend who will always believe in you" smile. It happens all the time. Potential love interests or just those friends who have complete faith in the protagonist usually do that smile.
If anything, I thought Tataru just triggered a death flag for herself with that smile because she was one of the constant things that (I assume) the WoL appreciated as part of the job, and it would have been really tragic if she was taken away from his/her life. I was pleasantly surprised when I found out she survived at the end of 2.55.

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