No. 1: Live and Let Die very closely followed by Dr. No through The Living Daylights.

Licence to Kill and the Brosnan films a bit less.

The OT and 97 SE

Everything else is pretty equal, but here's some other contenders:

Maltese Falcon, Casablanca, Treasure of the Sierra Madre

Man with No Name trilogy

Citizen Kane

Raiders

Blade Runner

Dr. Strangelove

Bridge on the River Kwai-Lawrence of Arabia-Doctor Zhivago

Vertigo, Notorious

The Godfather

The Third Man

Chinatown

and I could go on forever...