As above, NFS III: Hot Pursuit, PC Version, mixed with some good mods from NFSCars.
There's something unique about this game I miss. When I see the autumn leaves of Hometown or the magnificent futuristic race of Atlantica, I... I don't know. Yeah I think NFS Hot Pursuit 2010 was maybe the last one giving me this authentic NFS vibe, but I can't really say that for sure because I didn't really play the others. I honestly don't understand why EA need to stick with these cheesy scenarios. Enough of american block-busteresque humans behavior. Give us Cars, Ambiance, fresh UI Aesthetic (NFS HP 2010 was great on this point), memorable Races...
So, yes, NFS Hot Pursuit 2010 was good, but in terms of gameplay and handling, it felt more like Burnout Paradise had a children with Outrun.
Oh, and Porsche Unleashed was unique. One of the bests NFS too. High Skates wasn't bad either. And I need to play Hot Pursuit 2. The PS2 version seems to have a particular cars handling.