Specifically, my thoughts are on the selection of episodes (basically the only thing to gripe about with these releases, since they don't include any extras). The episodes chosen for the first volume more-or-less made sense: the two-part Borg blockbuster "The Best of Both Worlds", the masterpiece fan-favorite "Yesterday's Enterprise", and the most arguable of the bunch (but still excellent by any means), "The Measure of a Man".
As with any top-ten list, the further away from Number One you get, the more questionable the selections can become, so in that respect it's almost inevitable that the choices for volume two don't stand up quite as well to scrutiny. "The Inner Light", which probably should have usurped the spot taken by "The Measure of a Man" on volume one, is of course fully qualified to be there. Unfortunately, it goes downhill from there (although we are talking Star Trek: TNG, so it's all relative); they seem to have given more credence to the guest stars appearing in each given episode than to the actual quality of the stories. I don't have much problem with the choice of "Tapestry", because I like Q and it was one of the better Q outings, and I've always had a soft spot for good ol' Scotty, so you wouldn't get much complaint out of me for "Relics", but the fact of the matter is that there are plenty of episodes with more enthralling and well-written stories than these two.
The real capper, though, is that this disc's lineup of episodes is rounded out by "Cause and Effect". Are you kidding me? "Cause and Effect"?!? I mean, sure, it was an interesting premise with a decent story, but on my better days (today not being one of them, but that's off-topic) I can think of a good seven or eight episodes, off the top of my head, that would be more suited for a disc calling itself "The Best of Star Trek: The Next Generation" volume two ... or even volume three, for that matter. I have to wonder if the simple presence of Kelsey Grammer (who, by pure coincidence I'm sure, has a role in the moderately-anticipated remake of Fame that's about to hit theatres) is what bumped this episode into favor. We all loved Jimmy Doohan, so I'll let "Relics" off easy.
So, after looking at a list of episodes, here would be the lineup I'd have chosen for "The Best of Star Trek: The Next Generation" volume 2: "The Inner Light", "Darmok", and "Unification" parts 1 and 2. For volume 3, you ask? Let's see ... I think "Half a Life", "Loud as a Whisper", "Symbiosis", and "Hollow Pursuits". Of course, we could mix-and-match those, for anyone who might object to one whole volume being taken from a single season. And then there are some of my personal favorites, like "A Matter of Time", "Thine Own Self", "The Chase", and "Suddenly Human" ... that would be volume 4. I'd better stop here, 'cause I could go on for hours.