Goldfinger ★★★★★

The third film in the franchise had a budget that was more than the combined budget for the first two Bond films and it shows. Everything is ramped up and improved from Dr. No and From Russia with Love. 
Better villains, more women, better gadgets (the car), great theme song, a more convoluted plot, and a granny toting a machine gun. 
I’m not sure if it can get any better than this entry seeing as the bar has certainly been raised high. 

Spoilers: 
The scene at the end when Goldenfinger flies out of the broken window of the plane is probably the best thing I’ve ever seen.