Def. spend a couple of days at poko - right all together are PT Pillar, Gamesmanship, Bloody Mary, Fastest Gun and Green Onion.
I guess you can walk in to Wallface and do a route (you can do in and out in a day, no problem, with days being as long as they are) just to do it - honestly, it's not a place that I feel the need to make a habit of hiking in to, but it's something to experience at least once.
Hurricane has a few nice climbs - Quadraphenia was great; Forever Wild is beautiful.
If you can find directions to Willsboro, there is some one-pitch but very scenic (directly above the lake) climbing there. see, e.g. this photo: http://www.jimlawyer.com/Picture%20-%20WindJammer-LakeChamplain_WH12.htm?picring=2
- a little different than most of the rest of the High Peaks area.
Definitely go to Barkeater Cliffs. There is a lot of (mostly single pitch) stuff there, but some really beautiful climbs. It's nice because it gets away from the roads, which seems to be the problem with most of the other well developed crags in the area. It might be more moderate than what you're looking for though - mostly 5.8-5.10ish. I really liked Eat Yourself a Pie and Mr. Clean in particular.
To really pump yourself silly, go to the Spider's Web. All beautiful overhanging cracks, nothing really much easier than solid 5.8. For easy access, you can't really beat Pitchoff Chimney Cliff, and it's unfortunate that Rt. 73 runs right by it, because there are a lot of really stellar routes there (The El is a mega-classic moderate). I don't know that I'd personally bother with the Beer Walls. I think that there's just so much more that is more scenic - where you really get up and above and get a real feel for the High Peaks - rather than staying down in the canyon.
Honestly there is just soooooooooooooo much rock there that it's hard to recommend anything.
There are plenty of free places to stay besides Poke-O, just check the guide book - though if you're climbing at Poke-O, it'll be easiest to stay there since it is a little bit removed from most of the rest of the climbing in the area. I always recommends dinner at the Carribean Cowboy in Lake Placid, and breakfast is usually good at Cedar Run in Keene (73 and 9N are the same thing through Keene, Strat... Cedar Run is just before the two diverge as the reach the Ausable), although sometimes on weekends it can be slow and disappointing. Generally the disappointing can be avoided by ordering one of the wraps or breakfast sandwiches rather than an omelette... $5 pints of margaritas at Desperados in Lake Placid are also always a good bet.
Gear shop = the Mountaineer in Keene, or EMS in Lake Placid. I may work for the latter, but I'd go to the former.