Whenever I press the play button on Origin, it stays pressed for a few moments then goes back to being orange, with the launcher not opening. I can't get the game to open without the launcher from ProgramFiles, either. I've tried re-installing, removing my mods folder, and deleting my cache files. Can anyone help me?

You are on the Windows version of the game and not Mac? An Origin controlled game on Windows cannot be started without Origin and its hand-off to the Launcher, such is the magic of Patch 1.69. There are some relatively simple steps to follow when this happens potentially involving reinstalling Origin itself, clearing Origin's cache, and (this is new) disallowing a couple of services that might be getting in the way. I don't have them memorized though or know in which order to apply them as I've been on a Steam install for quite a while now. The folks here will know what to do.
https://answers.ea.com/t5/Technical...bd-p/the-sims-3

Yes, I'm on Windows, I wouldn't be caught dead with an Apple product. I've tried reinstalling Origin and clearing its cache, those haven't worked either. Do you know what services I need to disable that would cause this?

I do not know, sorry if I wasn't clear enough on that. Colleagues on EA's AHQ board do know because they help players who get stuck on Origin (usually after a recent update) all the time after seeking more information about their install, they know what to try next if just switching the services off doesn't fix it, and I gave you a link to the forum to post the question on. I wouldn't want to give you the wrong answers no matter what your personal feelings are against the Mac on which I am typing out these responses.

Alright, I'll try asking there, thank you. And I won't knock your preference for Mac, I just really detest Apple's business practices. Less features, higher price tag...