I've seen a couple of my choices listed already, but if you're looking into Child of Eden for PS3 (Beautiful game, I love it), go with Rez too. It's made by the same studio, ect. I emulate it myself and it's pretty easy to run even for an older machine, plus it's a quick download. I haven't seen Grim Grimoire listed yet, I started playing that last night and I'm enjoying it a good bit. And like some other posters said the Persona series is great. If you have a PSP and have it homebrewed you could download Persona 3 Portable for it. Way of the Samurai is also a pretty cool game, same goes for about any of the Tales of games. Then you have Metal Gear Solid if you can run it and Rogue Galaxy. PS2 has A LOT of great options. Oh, and Max Payne is great too.
As for PS3, to me Borderlands 2 is just not as fun unless you're playing with somebody else regular. I personally don't like the game, I found it a little too repetitive overall. If you have the money at the time, you can get Journey off PSN, that game is amazing. Then Tales of Xillia is soon coming to NA and I'm going to assume Europe too, so look out for that if you enjoy any other Tales games. I'd tell you to get Tales of Vesperia, my favorite Tales of game, but the PS3 release is still only in Japan if I remember correctly. You also have the Shadow of the Colossus/Ico collection for PS3, some great oldies that are also on the PS2.