Excluding George Lazenby for obvious reasons, I’m going to go through each of the James Bond actors and we can decide which is the best film for each actor.
From Russia With Love edges out Goldfinger by a hair. I like the fact it’s less jokey and gimmicky. Plus it has two great villains: Red Grant and Rosa Klebb.
My favorite is Diamonds Are Forever, but the best Bond movie is Goldfinger.
Had to go with Goldfinger…and I see the poll is anonymous…is that so when one Doper saunters in and votes for Never Say Never Again they won’t be ostracized? 
I think From Russia with Love was the best made Connery Bond film. All of the others were flawed in performance, story, or production.
Bond movies have achieved flaws in all fields of human endeavour…EXCEPT CRIME!!
Goldfinger is one of the few Bond movies I think holds up really well.
In a tough choice between Goldfinger and You Only Live Twice I pick the latter by a hair, probably in part due to Little Nellie. Every Bond film with Connery was awesome, both to a young impressionable mind and even in multiple replay over the years.
I just watched From Russia With Love over the weekend, and damn, is it a good movie. Karim Bey, the gypsy fight, Robert Shaw stole every damn scene he was in. And the fight in the train was incredibly well done.
Goldfinger is my favorite, hands down. From the “Welcome To Miami Beach” scene with the guy diving into the Fontainebleau pool to the car chase in the Swiss Alps to Oddjob’s deadly frisbee bowler to the “I expect you to DIE” line, it’s a movie I can watch over and over again.
Anyone not choosing Goldfinger has clearly never watched it.
It’s really hard to pick between Goldfinger and From Russia With Love. Along with RealityChuck, I liked the feel of Russia, so I chose that. I didn’t care that much for Diamonds, but I do think Jill St. John was IMHO, the best looking Bond girl of the Connery films. (YMMV, obviously.) Though Andress’s bikini scene is iconic, and helped cement the series in popular culture.
Goldfinger. Right mix of serious and humor, great villian. Props to Robert Shaw and Lotte Lenya for great villains in my runner up From Russia With Love.
For all those with great gushing love for Goldfinger, you do realize that it portrays Bond as being terminally incompetent, right?
For the count, Bond is:
[ul]
[li]Almost killed three times (pre-title sequence, on the laser table in Switzerland, in the depository fighting Oddjob)[/li][li]Captured/incapacitated four times (in Miami after forcing Goldfinger to lose at gin, in Switzerland at the foundry, by Pussy after the briefing to the Mafia, again by Goldfinger in the jet)[/li][li]Gets both Masterson sisters killed (Jill in Miami, Tilly in Switzerland)[/li][li]Fails to get a message out to MI-6 or CIA after he uncovers Goldfinger’s plan (courier is killed and compacted by Oddjob)[/li][li]Completely prangs up his Aston-Martin DB-5 despite being equipped with smoke screen, oil slick, machine guns, bulletproof glass, and ejector seat) and totally fails to escape due to driving into a building[/li][li]Fails to disarm the bomb (disarmed in the last three seconds by a CIA technician)[/li][li]Defeats Oddjob virtually by accident (electrocution due to Oddjob’s hat being embedded in the bars and a power line being severed)[/li][li]Defeats Goldfinger only by accident (stray shot blows out a window, Goldfinger sucked into “outer space”)[/li][/ul]
In fact, the only thing Bond genuinely succeeds at is blowing up the heroin processing facility in the pre-title sequence, cheating at golf, and seducing Pussy Galore from her man-hating lesbian (implied in the film, explicit in the novel) into betraying Goldfinger. (In reality, she probably realized how dangerously unstable Goldfinger was and how she and her circus were likely to be dispatched before receiving her reward, and opted instead to switch sides.) Bond nearly fails at every other task in the film. No wonder M is always threatening to send 008 to replace Bond. Goldfinger could be turned into a Rowan Atkinson film by changing a few names. The film has an iconic Shirley Bassey title song and some classic Ken Adam set design, but in every other sense it is absurd.
Now, let me tell you why Dr. Jones should just stay home and grade term papers…
Stranger
Yet his persistence prevails over all these setbacks. These are reasons that it is superior to Bond as an invincible superman. The hero must overcome adversity that appears to be beyond him.
I gotta go with From Russia With Love. Robert Shaw and Pedro Armendariz make that film what it is. Not to mention one of the most smoking Bond girls ever, Daniela Bianchi.
Well played, sir.
He causes most of these “setback” through incaution, indifference, and at times unbridled incompetence. If he had just followed Goldfinger to the foundry, overheard the conversation with Mr. Ling, and informed the MI-6 or CIA to intercept the convergence of Mafia figures delivering components to Goldfinger’s Kentucky farm the bomb would have never made it into the gold depository. He succeeds not due to his own abilities but because of the equal incompetence of Goldfinger (who can’t resist showing off his elaborate diorama of Fort Knox before inexplicably killing them all off) and the duplicity of Ms. Galore, who is actually the real hero of the film. In fact, I quite suspect that “Pussy” was actually Catherine Gale on a mission to infiltrate Goldfinger’s organization in order to subvert the plan with full knowledge that the standard intelligence services would screw it up, which explains why she was replaced by Ms. Peel. (This also brings into question what Ms. Peel was doing in On Her Majesty’s Secret Service, but since that was not a Connery Bond it is not of interest for us here.)
Stranger
From Russia With Love.
Connery had hit his stride with the character and the movie fairly closely followed Fleming’s novel. Probably one of the top three movies in the whole franchise.
And oh my stars, Daniela Bianchi was just a total babe in that movie.
either Goldfinger or From Russia With Love
Never Say Never Again shouldn’t be in the poll it’s not even a real Bond movie