Having played the PC and PS3 versions, I'd say they both have their pros and cons. The PC version, essentially being a straight PS2 port lacks some of the more advanced geometry and lighting effects of the HD remasters (since they are based on the then-graphically superior GameCube version).
On the other hand, the PC version can be forced to run in 1920*1080 and the likes, greatly reducing the aliasing present in the lower res PS3/X360 versions.
So graphically, the PC version (unmodded) looks slightly flat and bland, but you could argue it makes up for it with support for higher resolutions.
The Xbox 360 controller is supported and works great, but you need a mod to replace the button prompt icons with those of the controller, else they just show up as generic gamepad buttons.
And yes, the PC version is moddable to hell and back, but no matter how much you mod it, you won't get the more sophisticated visual effects of the HD rerelease.
I would personally lean towards the PC version since I can't stand jaggies and playing the console version on my 1080p TV made them noticeable enough for me to be annoyed by them. Maybe if you're on a 720p display they won't bother you as much, and the console version obviously is the more convenient one, even if the PC dito isn't as bad as some people make it out to be.
In the end, it's more or less a toss-up between the different versions, and a great game whatever your choice of platform.
EDIT: Forgot to add that if you go with the PC version, be sure to apply the official update available. Because out of the box it's not only by far the worst looking version of RE4, but nigh on the worst looking game of all time. :)
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