I've been using VLC for quite some time now, and I'm very happy with it. There is, however, one platform I'd like to see supported:
The Playstation 2.
I've had a harddisk in my PS2 for a while now, and the ability to run programs off of it is great. If a VLC port was to pop up I'd be more than happy - especially if it had samba support (so I could play files from the network directly like the xbox does).
I'm not a developer so I don't know how difficult it would be to properly port the software - but it sure would be nice...