This isn't really a New Frontier VS. Gotham Knight competition, so that should settle it.
I loved the animation of Deadshot, but I felt it was too short. Since producers touted him as the "anti-Bruce Wayne", they could have done a lot to exploit that side of his character. His pleading to Batman at the end of the one-shot felt uncharacteristic. "Crossfire" had that "Oooh, it's BATMAN" moment, which was great, but the rest was a little wordy. The rest is not memorable for me to review.
I agree with Malpractice. "Working Through Pain" was the most engaging and poetic/reflective episode of Bruce. It said a lot without saying too much. The image of Batman holding all those guns in the sewer is what stayed with me from this DVD.
As for the extras, the commentary was standard, and the Bob Kane story was great.
What I was disappointed with was the 4 episodes they chose from BTAS. The only one I would have kept was Heart of Ice. "I am the Night" does flow along the lines of Bale's existentialistic outlook in Begans and The Dark Knight, but it doesn't change how much I absolutely despise that episode for its (nod to Mike and James) "Hot Topic" reasons. Since they chose "Over the Edge", which included characters that weren't yet introduced in Nolan-verse, they could have gone with much better episodes such as "Almost Got 'Em", "Perchance to Dream", or "Read my Lips". Or include that "lost episode" of BTAS. Or include a NEW commentary. It would have given fans a treat.