@itstoriduh @pixiedust222 and @gre3nleaf I've merged all your posts into one thread because you all have the same error, not only that Sims 3 won't open but the CLR20r3-related crash of the launcher .exe. In case anyone's curious, CLR = common language runtime, i.e. .NET, and 20r3 is Framework 3.5.
For the two of you that haven't tried it yet, please uninstall and reinstall .NET 3.5; I'll repost what I wrote earlier in this thread:
Please uninstall (if already installed) and reinstall .NET Framework 3.5. Hit Windows key-R, enter "appwiz.cpl" without quotes, and in the window that appears, click "Turn Windows features on or off." .NET 3.5 will be right at the top. If the box next to it is filled in, it's already installed; click it to uninstall, wait for it to finish, and restart your computer. Then repeat the above, except click the box to install the framework, then restart. If .NET 3.5 is not currently installed, just install it and restart.
If that doesn't help, and @itstoriduh I know it didn't help, please try uninstalling and reinstalling VC++ 2005 x86, which Sims 3 uses. Your Reliability Monitor report lists a few different attempts to reconfigure this runtime, and Microsoft released an update for it this year. Sims 3's installer would necessarily include a much older version, and it's possible that either the game isn't compatible with the newer version or that a fully updated Windows isn't compatible with the older version. Either way, it's easy to test.
Hit Windows key-i, select Apps, scroll down to the Microsoft Visual C++ 2005 Redistributable, click on it (it's the x86 version but won't specify), and select Uninstall. Don't touch any other versions, including 2005 x64 if you happen to have it. Then install the newest one from Microsoft:
https://www.microsoft.com/en-us/download/details.aspx?id=26347
You only need the x86 version, not the other two. Restart your computer and try to play.
If the launcher won't open, please repeat the above, but this time, instead of using the updated runtime from Microsoft, install the older version that came with Sims 3. Open the installer within the game's program files, by default located here:
Program Files (x86)\Origin Games\The Sims 3\__Installer\vc\vc2005sp1\redist
Right-click on vcredist_x86.exe and select "Run as administrator." Once it's installed, restart your computer and try to play.