Yes, a Cold War thriller, dangerous with just enough 007 to avoid ruining it. From Russia With Love (as well as Dr. No) set the benchmark for what Bond should be, not Goldfinger or Thunderball. Both were classic '60s spy thrillers with terrific villains: Red Grant and Julius No. The girls are still some of the series' best Tatiana Romanova and Honey Ryder. Sorry my answer was a bit of a cop out, but I honestly am not sure which film I prefer: Dr. No or From Russia With Love. Admittedly, for the Orient Express and beautiful Turkish setting, I'll give the (slight) nod to FRWL.
So going along with that, I'll ask everyone else:
Dr. No
OR
From Russia With Love
?