Some of this depends on what kind of James Bond we're looking for.  If you want James Bond as Ian Fleming conceptualized him in the books, you'd go to Daniel Craig and then Sean Connery.  Fleming's Bond was cold-blooded and, at times, brutish.  He was not some smarmy, wooden hero who succeeded in outlandish or far-fetched ways.  That's what James Bond was made into by the Roger Moore movies and it's been tough to dig him out of that mold. 

Remember, Craig's Bond has just achieved his Double-O status, so this is James Bond before we come to know him in the Connery films.  In other words, there's still the possibility that the sophisticated yet ruthless secret agent we recognize in Sean Connery is being developed as we speak, by Daniel Craig. 

Brosnan was great in Goldeneye and The World is Not Enough, but Tomorrow Never Dies and Die Another Day I just don't think were that good.