daijawayout Cache files reappear; that's the point. They exist to store data an app can call on rather than recreating it from scratch, but that data can also get stale. Deleting them isn't meant to keep them away but to force whatever app is using them to generate fresh files with new data.
Options.ini stores all your in-game options, so don't delete that. The rest can be deleted with no harm done, but the cache files you're supposed to delete when adding mods or custom content are the five with Cache in their name.
For now, please move your Mods folder to the desktop, delete the cache files again, and see whether you can play. If the game works, please list the mods you installed previously. You can post a screenshot of the folder that contains them to show their names if it's easier.
If the game doesn't work, move the entire Sims 3 folder to the desktop and try again. This will remove, but not delete, your saves and other user data, all of which can be restored later.
