All the big multi-platform games are on here already: BioShock, Mass Effect, Ninja Gaiden, Dark Souls, Catherine, and even Deadly Premonition is getting an updated version. All the big-name stuff; Tomb Raider, Portal, Batman, Elder Scrolls, and even Ar Tonelico! Here's what I can list off the top of my head:
Exclusive
Uncharted 1-3
Resistance 1-3
Disgaea 3 & 4
Hyperdimension Neptunia 1-2
Ratchet & Clank Future Trilogy: ToD, QfB, CiT
Heavy Rain
Heavenly Sword
God of War HD Collection
God of War 3
Sly Cooper HD Collection
Ico & Shadow of the Colossus HD Collection
Jak & Daxter HD Collection
Little Big Planet 1-2
Tales of Graces F
InFamous 1-2
Metal Gear Solid 4
Killzone 3
Mugen Souls
Coming Soon to PS3
Sly 4: Thieves in Time
Ni No Kuni: Wraith of the White Witch
Deadly Premonition
The Last Guardian
Time & Eternity
Monster Hunter
PSN
Odin Sphere
God Hand
flOw/Flower/Journey
Final Fantasy 1-2
Final Fantasy 4-9
Xenogears
Chrono Trigger
Chrono Cross
Wipeout HD
Siren: Blood Curse
Blue Toad Mysteries
Metal Gear Solid
Resident Evil 1-3. RE4 HD.
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You can't go wrong with those. There's plenty more titles, and I'm a happy gamer! The PS3 isn't exactly hurting for software. Welcome, and good luck!