I don't think it would need to be moved onto your local PC, leaving it on the network should be OK for now.
I would do the following -
Unmonitor the network folder in the Zune Software via Settings.
Close Zune.
Reset the software library by doing the following:
1. Navigate to the following directory (OS Specific):
a. XP: %homepath%\Local Settings\Application Data\Microsoft\Zune
b. Vista: %homepath%\AppData\Local\Microsoft\Zune
2. There should be a file of your library called zunestore.sdf
3. Rename the file to zunestore.bak
OK, relaunch the Zune software. At this point, you will either have no library or whatever content you have in the default music locations. Remonitor the network location and wait for the music to reappear in the Zune Software Library.
Attach device. You should get a prompt of some sort that the device is associated with another computer. You may only see this in device settings. I suggest connecting as a guest. Once all that has happened, go ahead and try syncing your content again, but you'll have to do it manually, you can just drag n drop from within the Zune software onto the device icon.
Let me know if it works... I will check in again on Monday.
gina / Zune Software Product Team / This posting is provided "as-is" with no warranties, and confers no rights