Firstly, it's worth noting that this works out cheaper than most of the Buy One Get One Free offers on the Bond Ultimate Editions at the moment. It contains all 6 Connery Bond films in there Ultimate Edition 2 disc formats.
There is, it should be noted, a gap between You Only Live Twice and Diamonds are Forever where On Her Majesty's Secret Service should be... (which of course featured George Lazenby so shouldn't be included here).
Here you get Bond at his best, but the fact that you're already looking at this means you know that! The picture on these Ultimate Editions is truly something to behold. In certain sequences in Dr. No and From Russia with Love I could have sworn that I was watching a film shot a few years ago set in the 1960's. That's not an exageration. It's probably the best restoration job I have ever seen. I upgraded from my old Special Editions and I honestly believe it was worth it just for the picture.
If you have the old Special Editions... the extras are replicated here along with a few additional bits and pieces. Is it worth upgrading? If you're after improved picture and sound... yes... if you're a huge Bond fan... yes... but if you're a casual fan, already possessing the Special Editions and not that interested in improved picture quality... no.