I voted for Casino Royale and No Time to Die because they're the two I remember best (and the latter one because I just saw it, LOL).
Simon wrote:
I honestly wasn't thrilled with any of them. It could just be me or the age I am...but none of them felt like they approached the greatness of Sean Connery or the fun of Roger Moore or even the oddly nondescript likeability of Timothy Dalton or Pierce Brosnan.
Barry Nelson was an early TV bond and not part of the movie franchise proper, and George Lazenby was just a minor one-shot entrant in the franchise so it's hard to really comment on him. David Niven was a comedic parody of Bond so he doesn't count, IMO.
I like all the Bond films except Roger Moore's. Even the "good ones," like For Your Eyes Only and The Spy Who Loved Me are tedious for me to get through. I don't buy him as a government super-spy / assassin and the movies are campy, which I usually like, but his films are not campy in a way I find entertaining. It's a shame, because I actually really like Roger Moore as an actor and a guy, he seems really cool and very nice. I think he'd be great as "M," but I don't buy him as 007.
I LOVE Connery, he's clearly the ultimate for the role. I thought Lazenby was very solid (tho I wish Connery could have done that one TBH), and I like Dalton and Brosnan, but the only guy who came close to Connery in my book is Craig. All the Bonds from Moore to Brosnan have the suave, dapper thing down pat and I can buy them as seductive leading men, but I can't believe them as stone-cold killers who can kick ass. Connery and Daniel Craig made Bond seem like a tiger in a fitted suit -- they bring an element of danger, an edge, that I think the character needs. I think it should feel like MI6 found a kid with a killer instinct and taught him how to pretend to be a suave high-society gentleman -- not like MI6 found a high-society gentleman and taught him how to be a killer, if that makes sense.
Simon wrote:
I'd have to say Casino Royale because it was the most Bond-like entry Craig starred in, I think. They weren't trying to 'reimagine' anything at that point, just introduce a new Bond. Messing around with the core concept came later. I also like the villain(s) and the action sequences in Casino Royale so that one gets my vote.
I think your memory is playing tricks on you, my friend.

They were totally trying to reimagine the Bond franchise at that point, most likely in response to the success of the Bourne and Mission Impossible movies. The last Brosnan one was a campy mess, the only highlight was Halle Berry's incredible looks, and it was borderline Schumacher territory. Casino Royale is a Batman Begins style reboot that went the other way, with an emphasis on gritty violence and dangerous people. No more Bond killing a room full of guys with only a few hairs out of place to show for it, now he was bruised and bleeding after every fight. Q wasn't even in this one and there weren't all the usual fancy gadgets and sports cars with machine guns.
Beyond that, the movie also delved a little more into Bond's psychology, questioning the mental state of a man who goes into this line of work. They really played up the tragic nature of the character and if anything, I'd argue the last 2-3 films were the ones that brought Bond back to the platonic ideal -- eventually they brought back Q, the suped-up cars, the gadgets, and all the other tropes of the franchise. But Casino Royale was where they broke with the classic 007 formula established in Goldfinger.