Everyone has their preference, but safest bet is probably Cosmic Genesis. But all the Mr.V albums are good... can't go wrong. My personal favorite is Visions from the Spiral Generator, but my favorite song, Microscopical Macrocosm, is on The Focusing Blur.
It seriously is a good discography, though. So getting everything is something you should consider. I say that as a fanboy, but most people would agree that if you like Mr.V's stuff, he has been consistent about quality in his recordings.
And if you're not someone who cares about having the physical CD (I'm not), you can get most / all of them on iTunes (haven't checked for all of them, since I physically own all my Mr.V CDs).