I'm not much of an overclocker, so I don't know hardly anything about the process.
I'm looking to bump my 4850 up enough to run Crysis on Very High, and I was wondering if someone could help me out with the values I need to enter in CCC.
Yeah I think the GT was pushing the GTX hard at low res.. It was at mid to high res that the GTX was still king over it due to the higher memory and bandwidth.
To run Crysis properly at VH settings at 1440-900 you'll need at least a HD4870 or GTX260 or higher. Crysis doesn't really improve much when increasing/decreasing resolution due to bad optimizations (which I believe is fixed in Crysis Warhead).
If you want to run it on VH on a HD4850 then I suggest overclocking the core to around 700MHz and the mem to around 1100MHz and to keep safe temps perhaps buy a 3rd party cooler (I highly recommend the Accelero S1 or the upcoming T-Rad2). And download some Crysis tweaked cvars which improve Crysis's look visually whilst maintaining good framerates.