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Well, I don't know anything about the systems, but PSP is already obsolete and PS Vita is still in his Prime and has more potential

what you have in mind is very good at issue the portability

I googled and found this

PSP-Series - (1000 = 32 MB Ram), (2000 = 64 MB Ram) and (3000 = 64 MB Ram). with just this amount of Ram, won't tolerate the Unity engine

Agreed

Personally a port for the Nintendo 3DS makes more sense especially because Unity does 3D automatically (so you only have to worry about the controls) however the PS Vita port would be nice due having more power (less lag) and a longer battery life.