No, because if you use iTunes to sync the iPod, it won’t let you sync from a remote share.
For Firefly it doesn’t matter if you listen to the songs, or download them or whatnot. It will serve you the requested content.
But there are dozens of other apps that allow you to put music on your iPod. Like this app for instance.
I guess the chances are best that apps like Amarok or Rhythmbox will allow syncing even from a remote iTunes share.