Rondo would be cool, it's one of the few console ones I haven't played at all yet, along with Bloodlines.
They are both on VC though IIRC so it's not like people don't have access to them, which is usually partially the reason why remakes are done.
My vote would go for Simon's Quest. As someone before earlier said it, it needs a remake.
More than it deserves one, honestly.  
