A teacher here at school had the same issue on Windows 10 64bit ver. 20H2. I couldn't get into Settings because that merely opened a tab having the sad face. Uninstalling and reinstalling didn't work. But I was able to sign out as the teacher, sign in as the computer's admin, and all worked well. Only when signed in as the teacher did this problem occur.
SOLUTION: I went to this folder:C:\Users\user_name\AppData\Local\Google\Chrome\User Data
Then I deleted all files and folders contained in it.
WARNING: You'll need to save bookmarks because this process looses all personalization and user data. I had to set up Chrome from scratch just like I did when I first provisioned this machine for the teacher.
I hope this helps others.
Cheers,
Bill
