I don't believe it is possible.
The only way I think it could possibly be possible is if you have an iPod in disk mode (like an iPod classic), and made an alias to the iPod disk and put it in your movies folder.
Then, when you clicked on front row, movies, you would see your disk, and then be able to play media from there.
Downsides I beileve is that the 'disk' side of iPod, and the 'iPod' side of iPod are separate (I believe), so you'd need all your music (likely duplicated) on the disk side.