I use excel. I know Jeff uses (or did use) a program to scan his games into a document. Don't remember the name and don't know if it would sync with Steam.
I don't know of any that sync with Steam. If you later end up dropping that requirement, I really like Game Collector (http://www.collectorz.com/game/). I have used it for about 5 years and it works great. Fair price and tons of features, including exporting data to a phone app.
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