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Hoo, boy.
I've used Shelfari, GoodReads, LibraryThing and Readernaut. I've also got a trial Book Collector Connect account and have both Book Collector and Books installed on my MacBook while I try to figure out what I want to use.
Part the First: Cataloging. I'd love to have a definitive catalog of my books, preferably both on my laptop/desktop and online. That's one thing I like about the Collectorz.com stuff (Book Collector, the client app; Book Collector Connect, the web app): you can synchronize between their online app and the PRO version of their desktop app, so you've got access to your catalog (say, for insurance purposes) whether you can get online or not (or, on the flipside, whether your desktop and/or laptop was destroyed in the same fire, flood or other calamity as your books). The PRO version of the desktop application runs $40-50 and the online app is a subscription model and runs $10/year. (I have the PRO version of Movie Collector and a paid subscription to Movie Collector Connect.)
Part the Second: Sharing/Social Networking. The main drawback to the Collectorz.com stuff is that it's essentially just a big list of stuff and data points about that stuff. It's great for cataloging and good for showing off your collection, but there's no social component whatsoever. This is where the strictly-online services come into play.
Personally, I think GoodReads takes the crown when it comes to the social networking piece. Their main page is very similar to the news feeds (or "streams") you see on sites like Facebook and Twitter and whatnot: "Joe is on page 165 of THE DAVINCI CODE" and "Brenna gave four stars to LOVE IN THE TIME OF CHOLERA". I think Readernaut has a cleaner interface and some nice features (being able to upload your own cover images, for example), but it's just not as popular; when all your friends are on Twitter, it's tough to keep using Jaiku day after day.
LibraryThing has the most raw data about each book, but the social networking aspects are pushed into the background. LibraryThing also works on a try-before-you-buy model; allowing you to catalog something on the lines of 200 titles before asking you to pony up some cash.
I didn't care for Shelfari, because it seemed to be largely about showing off pretty graphics. I only knew one other person with an account there, so I didn't last long before I decided to stop using it.
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