I'm running all my emulation stuff off NAS right now, between CD images for my extensive collection of PSX/Saturn/SegaCD/etc discs, cartridge images for the consoles I've collected, and the images for the arcade boards I have. Unless you have gigabit ethernet on that NAS and don't mind it getting thrashed, you're going to probably hit serious problems with laserdisc images.
I'd suggest that you decide ahead of time on whether you're planning to let the stuff be accessed from multiple machines at once so you can set your MAME config(s) accordingly. As someone else here said, you really don't want to share your state directory if there's any chance of people overwriting one another.
I'm also using "USB Detect and Launch" in concert with Microsoft SyncToy to sync save data between an SD card I use on my Wii and netbook frequently and my main archives, as well as to a PSP memstick I have. If you have the inclination, there's a LOT you can do with small tools like this to make life interesting. I'm even syncing all my save data to Dropbox to have a backup on the "cloud" so to speak.
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Try checking the MAME manual at http://docs.mamedev.org
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