kerryc123 You may or may not be able to deselect subfolders within the Sims 4 user folder; I've heard mixed reports about the option in Windows 11. Right-click the cloud icon in the lower-right corner of your screen (or perhaps hidden in the Tray, the ^ icon), open Settings > Account, select Choose folders, and expand the subfolders until you find the ones you don't want synced.
Deselecting these folders will remove them from your computer and leave them only in cloud storage. So if you want to keep your current copies, it's best to make a backup of the folder(s) you're going to deselect first. You can restore their contents once you've changed OneDrive settings, and the files shouldn't be synced again. You can also delete them from onedrive.com after the fact, or download them from there if you forget to make a backup beforehand.
If you don't see this option, look around a bit to see whether it's hiding somewhere else. I'm still running Windows 10 and haven't tested OneDrive in 11 yet, so I'm not completely sure what options are still there.
If you can't find the option to deselect individual folders, let me know. There is another approach involving a symbolic link that might work, but it would be something of an experiment.