First, regardless of whether it is "safe" or not, removing the keys will gain you nothing.
Also, googling this was hilariously facepalm worthy with misinformation. ("Microsoft updated excel and because I sent in the spreadsheet for tax info without checking my macros from 1992 they can't be trusted" haha)
Basically, a tlb file is a "type library". In the case of .NET, these are generated for use as COM wrappers around .NET components.
the key here is "generated"; removing these keys won't really gain you anything since they are going to be regenerated when next needed. The difference is .NET will no longer know how many components reference it.
Now, it might not cause problems. But the thing is- leaving them there is not going to cause issues, so why tempt fate?
Sure can, if you want most of your .net applications to start having random issues.