For me, Modern Warfare. Ive been Playing World War 1&2 themed games for a while now (CoD2, Medal of Honor series etc...), so in campaign it was nice to be able to pick up a stinger launcher and wreak havoc, not to mention being able to use laser sights on guns, and being able to operate the turret of an aircraft.
Multiplayer was fantastic too, with the previously mentioned laser sights, and a diverse range of weapons i hadn't used before.
CoD4 brought with it an array of new things, whereas 5 had much of the same stuff.
Edit:
QUOTE (Redhatcc @ Feb 14 2009, 01:33 AM)

like to throw in.... the next COD is going back to Modern Warefare
Call Of Duty Modern Warfare 2
Awesome as! Cant wait.