I can highly reccomend Dr No.
The blu-ray is STUNNING. It almost looks like it's been filmed recently and just happens to be a 1960's period drama.
I suspect that the other Bond movies out on Blu-Ray are as good. According to the "making of" documentry on the disc they went back to the original camera negatives, then scanned them at a resolution of 4k (as in 4 times the vertical resolution of 1080 HS), a resolution which is ever so slightly higher than the grain resolution of the original film, so they captured everything, then they basically re-edited it and colourbalanced it scene by scene and digitally removed any film tears and scrathes etc.
They did the whole series for the DVD box set, but they planned ahead of time and did it at 4k resolution, so there'll be decent quality copies of bond films for DVD, Blu-Ray and whatever comes after it.
edit: Also, as almost everyone else points out, Dark Knight is amazing, the IMAX shots are insane. Planet Earth as well. Great Sunday afternoon viewing