I know it's kind of obvious, but Xenogears and Xenosaga are the first one's I'd go for. Both very similar thematically, as you might expect.
Xenogears second half is a bit disappointing but still an excellent game. Story gets a bit crazy but if it's more Xenoblade you're looking for that should be a plus. Xenosaga is even more insane (I recommend the Perfect Works Translation) alongside/after playing the three games though, as the story and concepts discussed get utterly impenetrable.
Vagrant Story is excellent but not exactly a traditional JRPG. Really interesting crafting and levelling system. You gain resistance to healing from healing yourself too much, so if that sounds neat I'd definitely recommend giving it a try. Holds up surprisingly well visually as well.
Shin Megami Tensei: whatever is also a great choice. Nocturne, Digital Devil Saga 1 & 2 for more traditional, or Devil Summoner for more action based combat. Also Persona, all excellent games.
Since I haven't actually suggested a ps3 game my choice would be FFXIII-2. I know plenty of people hate it (and XIII) but I absolutely loved it, and it was one of the few games I have 100% completed in years.
As far as acquiring these, Xenosaga and Vagrant Story are both on PS1 classics, Xenosaga is a bit hard to find (and requires buying three games). Some of the SMT stuff can found on the PSN (Persona, P3) and the rest are not too hard to find on Amazon and the like. Not the most popular games in the world so you can even find new copies for <$30.
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