Tried removing the gta_vc.set file located in Vice City User Files folder? Besides, your problem is similar to this:
|Problem:Vice City periodically locks up with the sound still playing.|
Solution: Disable custom MP3s or take a look at file names - it seems the game dislikes huge filenames for MP3s (e.g. "01 - Artist - Album - Song.mp3").
Alternatively: Re-install the game with the optional 'radio stations'. This means the game will run solely off the hard drive, thus giving better performance on most machines (although worse performance on older machines).
Alternatively: Roll back your drivers - the new nVIDIA drivers apparently aren't the best for use with Vice City. nVIDIA drivers version 61.76 are recommended.
Any of them help?