I Know now of at least 3 I am taking over, (taking all 21 that I have of course)
*Goldfinger - Its a classic SC Bond film and its doesnt have SPCTRE as the main opposition whic is good if you aren't watching in a specific order which I am not planning on.
*Live & Let Die - Roger Moore's first and a good film, it has the weird creepy Vudoo and things of that nature which may connect with him on that "Fringe" & "Lost" level.
*License to Kill - I love Timothy Dalton (so shoot me with the golden gun) and I find this film to be fairly decent and it has 007 going semi Rogue.
Clearly there is just so many to choose from
I may consider TSWLM, GoldenEye, Casino Royale, & FRWL
everything else is also a consideration