I am approaching my Google Drive limit, and Gmail uses 8GB. I found some photos with large attachments via filtering by size.
If I add these photos to Google Drive > Google Photos, will they stop counting against my quota?
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Your storage space is shared between Drive, Gmail and Photos anyway, so in general it doesn't matter which of them contains those pictures.
But if you upload via Google Photos' webpage and/or use Google Photos/Drive's sync app (it's now the same app for both of them), and choose (only) High Quality, that reduced quality will entitle you to unlimited image storage.