@Abi_tumblree Program files are read from your hard drive, not from OneDrive; having a second copy within OneDrive does nothing except occupy space. The game would not only be playable without OneDrive syncing the files, updating would be a lot more efficient.
It actually sounds like you've listed the synced copy of TS4_x64.exe, as in, the search found the one inside OneDrive, and the original is on your desktop. That's not the best setup just by itself: it would be better to have the game installed somewhere within Program Files (x86). You can of course leave it on your desktop, but for various reasons (including but not limited to the ability of OneDrive to sync your desktop data if you want that feature), I'd recommend moving it.
In order to do so, the first step is to completely disable OneDrive. You can reenable it later, but for now, get it out of the picture. Restart your computer, open your Origin game library, right-click on the Sims 4 icon, and select Move Game. From there, select This PC > C: > Program Files (x86) > Origin Games as the destination, and let Origin move the game's program files.
Once you've done that, you can reenable OneDrive, but be sure to delete whatever Sims 4 program files are in cloud storage. Or you can leave OneDrive disabled: it's not necessary for anything really, and many of us never use it. If you do want it running, I'd recommend preventing it from automatically syncing Documents at the very least, as this can interfere with your saves and other user content.
https://support.microsoft.com/en-us/office/choose-which-onedrive-folders-to-sync-to-your-computer-98b8b011-8b94-419b-aa95-a14ff2415e85