Well, I tried using Rowmote with VLC but it didn't really work…*I could control the sound level and I could choose previous & next, but the pause/play button didn't do much.

(I believe/hope updates will fix this "soon").
I agree that iTunes Remote is good, and I'm using it as well.
I actually have all these apps to make my "remote controlled environment" complete:
*Air Mouse - To control the mouse.
*iTunes Remote - control iTunes.
*Keynote Remote - control Keynote.
*Rowmote - To control & launch: Front Row, QuickTime (with Full Screen Toggle), iTunes, DVD Player, EyeTV, Keynote, PowerPoint, iPhoto, (VLC), Plex, Finder, etc…

*Jaadu VNC - EVERYTHING!