I've been reading through the Bond books (Bought all of them back in December), and I have to say I think that Sean Connery absolutely nails the part, and talks, acts, and looks (minus the scar) like I picture bond while I'm reading the books.
Brosnan, on the other hand, is also a fantastic Bond in my opinion, because he brings Bond into a more modern look and style, while still maintaining that classy attitude from the books.