Fallout intro. The vintage The Ink Spots's Maybe song playing as a background to those terrible images immidietely convinced me I just installed something truly incredible. 14 years later I still remember that very moment, so I guess the initial impression was spot on
Also..Return Fire (old game from 3DO) was awesome, because it was simplistic shotem-up with blowing everything up and that was accompanies by soundtrack of the biggest classical music pieces, like Flight of the Valkyrie, In the Hall of the Mountain King or Flight of the Bumblebee , which made for some really nice combo.
and while im sure the actual game gets a lot of hate, the way the music was a intricate part of the gameplay is by far my favourite use of licensed music.
All they needed to do is add the music control on top of the original mechanics rather than replacing them.