Crashes on Mainmenu

I'm not sure I entirely understand what you did. All I did was take my entire Saves Folder and move it out of my The Sims 4 Folder and onto my desktop. I then just started the game and it loaded. From the Main Menu screen, without creating a new save or anything, I re-enabled mods, applied the changes and closed the game. Then I put my entire Saves Folder back into my The Sims 4 Folder and the game started, all my saves were intact and everything has been fine. I didn't do anything at all with individual save files. If you did, maybe that caused an issue? 

In the first screenshot you have it shows the availability status as "Sync Pending". Could it be a syncing issue with OneDrive? Maybe there is a discrepancy and you need to sync. Check your recycle bins on both OneDrive and your Desktop and see if there are any files in there that maybe got accidentally deleted. I have OneDrive as well and it does not play nice with Sims 4. When I delete files, I have to constantly go into both recycle bins and also delete the files from there because OneDrive loves to take old files and overwrite newer files if you leave them sitting in the recycle bins. 

I also do feel like people that have removed their Saves Folder, gotten the game to load, but then created a brand new save file in order to re-enable mods (as opposed to just doing it from the Main Menu screen) also subsequently continue to have loading issues.