Not interested in the multiplayer component of either series and speaking strictly about the campaign, I enjoyed Crysis considerably more!
Call of Duty 4 (MW2 as well) is a well-crafted game for what it strives to achieve, among it's peers of similar style it's easily an above average and fun game. However, the linear/scripted style of FPS experience is more typical while Crysis offers more rich, unrestricted FPS combat in comparison.
I remember this comparison video that was done shortly after the games were released http://www.youtube.com/watch?v=gyQTCeobZlg
Crysis probably appeals less to the mainstream, which to a degree is unfortunate as there aren't many games that offer similar gameplay. I'd personally love to have another similar shooter, here's to hoping Crysis 2 and Far Cry 3 can provide some great emergent FPS gameplay!
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