Connery:
Best - From Russia with Love
Worst - Diamonds are Forever

Lazenby:
This choice isn't particularly hard.

Moore:
Best - The Spy Who Loved Me
Worst - A View to a Kill

Dalton:
Best - The Living Daylights
Worst - Licence to Kill

Brosnan:
Best - Goldeneye
Worst - Die Another Day

Craig:
Best - Casino Royale
Worst - Quantum of Solace

Connery:
Best- From Russia with Love
Worst- Dr. No

Lazenby:
I hate On Her Majesty's Secret Service

Moore:
Best- Live and Let Die
Worst- Octopussy

Dalton:
I like both, but would say I like The Living Daylights more.

Brosnan:
Best- Goldeneye
Worst- Die Another Day (though it has some nostalgic value for me)

Craig:
Best- Casino Royale
Worst- Quantum of Solace

Connery:
Best- FROM RUSSIA WITH LOVE
Worst- DIAMONDS ARE FOREVER

Lazenby:
Best- ON HER MAJESTY'S SECRET SERVICE.
Worst- N/A

Moore:
Best- LIVE AND LET DIE
Worst- A VIEW TO A KILL

Dalton:
Best- LICENCE TO KILL
Worst- THE LIVING DAYLIGHTS (though both are excellent)

Brosnan:
Best- GOLDENEYE
Worst- DIE ANOTHER DAY

Craig:
Best- CASINO ROYALE
Worst- QUANTUM OF SOLACE (though it's still solid)

Connery:
Best - Goldfinger
Worst - Diamonds are Forever

Moore:
Best - For Your Eyes Only
Worst - The Man with the Golden Gun

Dalton:
Best - Licence to Kill
Worst - The Living Daylights

Brosnan:
Best - The World is Not Enough
Worst - Tomorrow Never Dies

Craig:
Best - Casino Royale
Worst - Quantum of Solace

Connery:
Best: Thunderball
Wrost: Never Say Never Again

Moore:
Best: The Spy Who Loved Me
Worst: A View to a Kill

Dalton:
Best: The Living Daylights
Worst-License to Kill

Brosnan:
Best: Die Another Day
Worst: The World is Not Enough

Craig:
Best: Quantum of Solace (just lucky by sheer elimination)
Worst: Casino Royale

Sean Connery

From Russia with Love
Diamonds Are Forever

Roger Moore

The Spy Who Loved Me
Live and Let Die

Timothy Dalton

Licence to Kill
The Living Daylights

Pierce Brosnan

GoldenEye
Die Another Day

Daniel Craig

Skyfall
Quantum of Solace

Sean Connery

Best :Dr No
Worst :Diamonds are forever

I still like Diamonds but not as much as his previous 5 films bit still very watchable

Roger Moore

Best : The Spy who loved me
Worst: live and let die

Pierce Brosnan
best : Goldeneye
Worst :Die Another Day

Note: unlike most here, i love this film its just that from his 4 film DAD s is the one that i liked the least but that doesn't mean i don't like it

Daniel Craig

Best : Casino Royale
Worst: Quantum of Solace

Again i still like it but from the three we have seen till now is the one i liked the least but its still has its good moments here and there

Connery

Best: Goldfinger

Worst: Never Say Never Again

Moore:

Best: The Spy Who Loved Me

Worst: Live and Let Die

Dalton:

Best: Licence to Kill

Worst: The Living Daylights (still good though)

Brosnan:

Best: Goldeneye
Worst: Die Another Day

Craig:

Best: Skyfall

Worst: Quantum of Solace

Connery:
Best: Goldfinger
Worst: Diamonds Are Forever

Moore:
Best: The Spy Who Loved Me
Worst: Octopussy

Dalton:
Best: License to Kill
Worst: The Living Daylights

Brosnan:
Best: GoldenEye
Worst: Die Another Day

Craig:
Best: Skyfall
Worst: Quantum of Solace

I still have not seen them all yet.

Connery
Best: From Russia with Love
Worst: Diamonds are Forever

Moore
Best: The Spy Who Loved Me
Worst: Octopussy

Dalton
Best: The Living Daylights
Worst: n/a, haven't seen Licensed to Kill and TLD was great.

Brosnan
Best: Goldeneye
Worst: The World is Not Enough

Craig
Best: Casino Royale
Worst: Quantum of Solace

I didn't do Lazenby, since he only did one and I think his one is a top 5 Bond film, imo.

The films I have yet to see: Thunderball, Live and Let Die, A View to a Kill, For Your Eyes Only, Licensed to Kill, Die Another Day

Connery:
Best - Goldfinger
Worst - Thunderball (or Never Say Never Again if it counts)

Moore:
Best - The Man with the Golden Gun
Worst - Octopussy

Dalton:
Best - Licence to Kill
Worst - The Living Daylightd

Brosnan:
Best - The World is Not Enough
Worst - GoldenEye

Craig:
Best - Casino Royale
Worst - Quantum of Solace