The size of the Zune album art is 240 by 235 pixels in JPEG (.jpg) format. To update, right click on the album, select Update album art (Add album art when there is no image on Zune at all) from the menu, then choose an image from your computer.
The default Zune album art which provided by the Zune software is named as ZuneAlbumArt.jpg and stored as a hidden file in the folder of the music files. The customized image is named as ZuneCustomAlbumArt.jpg, also stored in the same directory.
If you want to edit the image, but can’t find the original or the one in the music folder, please make sure hidden files are shown, here is the tutorial: How to View Hidden Files and Folders in Windows Vista?
Hints: If the ZuneCustomAlbumArt.jpg didn’t show up on the Zune, cut and paste the hidden file to desktop, reopen Zune software, repeat Update album art, Zune software will put the ZuneCustomAlbumArt.jpg (make sure it’s 240×235 pixels) as a hidden file back to the folder again, and you should see the image on Zune this time.
The worse case, close the Zune software, disconnect the Zune, cut and paste the whole album (the folder which contain the music files and the album art) to a directory which Zune software is not monitored, such as the desktop. Reconnect the Zune, that album will be removed (assume Zune is monitoring the folder), close the software and disconnect the Zune. Copy the album back to the Zune monitored music directory, reconnect the Zune, it should open the software automatically. If the Zune didn’t pick up the album, you can drag the folder into the Zune software under the music collection.
The worst case, sell your PC and Zune, buy a Mac and an iPod. 
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