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At what resolution? Everything is a bottleneck for Crysis - how do other games run?
Your CPU would probably be a bit more of a bottleneck, but your system overall is pretty good.
Actually I could be way off. Anyway this site should help somewhat, I know they are testing with the 280 but thats not too far off your OC'd 260:
http://www.legionhardware.com/document.php?id=775&p=4
I have:
E6600 @ 3.3ghz
GTX 260 OC @ 666mhz core/1107 memory
4gb 800mhz ram
Is my GPU or CPU a bottleneck for crysis etc?
I would have to say that it is your CPU holding you back, regardless of resolution.
Since the E6600 runs stock 2.4GHz @ 266FSB, your OC of 3.3GHz is @ 366FSB
Have you tried to set it up to 400FSB 3.6GHz? Or considered a 45nm C2D?