Hard to say, the original VC is classic and has nostalgia, and great songs such as Missing You, Crockets Theme, or pretty much all of Emotion, and actually the whole soundtrack I love every song, Out of Touch, Video Killed the Radio Star, Pale Shelter, Kids in America, 99 Luftballons, Self Control, I Ran (so far away), Rock Box (Run DMC), the list goes on. And VCS it's the same situation, VCS has Easy Lover, The Warrior, Love is a Battlefield, Wouldn't it be Good, It's My Life, Relax, Space Age Love Song, I Want to Know What Love Is, I Can Dream About You, and of course In The Air Tonight which is to me the greatest song ever.
To me Espantoso is also better in VCS, I had some great atmospheric feelings towards the beginning of the game cruising around Little Havana during the day and Espantoso going. I always go Espantoso in the day and move to Flash or Emotion by night.
Very hard to choose, it's like choosing your favourite child. I'll probably say the original VC soundtrack, that is just perfect. VCS went for a more darker and neon tone to the whole style of the game, so that soundtrack is perfect too. I think I'll say the original VC though, maybe it's the nostalgia in me. Even though I feel like VCS has the stronger line up, my heart keeps saying VC.