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Does AO/AE look better on the PC?
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Yes, but only because there are no TV scanlines on PC version (you can turn them on for speed, though.... epsxe can turn them off/on anyway...) and so the game looks a little bit smoother... that's it
I think there is no need for buying PC AO/AE unless Paul rewrites game engine or whatever interesting else happens

In ePSXe you can also add some shaders (Pete's OGL2 plugin) and use some graphic filters for enhancing the graphics