I tried starting iSync to see if anything was new, and it would crash immediately. According to Apple's support site, deleting "/Library/Application Support/SyncService/501/*" (where 501 is your uid) would fix it, and it did. Unfortunately, iSync still crashes if I try and go into it's preferences or add a device. I tried it on another user account, and it appeared to work fine, so there must be something odd with my account. Looking at Apple's discussion groups, it appears that some other people have encountered this as well, but no solution as of yet.
While playing around with iSync, I tried plugging in my old 1st generation iPod to see if I could add it as an iSync device. I thought this iPod was pretty much dead due to bad harddrive sectors, but on a whim, I tried running Disk Utility on it, and it was able to correct an error (leaf record count in the catalog file). Then, I tried moving my MP3s over from iTunes and it didn't get hung up or anything like it used to. So, it appears that my old iPod is back from the grave. What's strange is that I had tried reformatting it's harddrive before, and that didn't work, which is why I was (and still am) sure it's hardware related and wasn't file system corruption.
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