A lot of documentation that needs to happen is for developers... I have reworked the order status API and the checkout pane API and don't know that I've documented it. Also, I'm about to dive headfirst into the line item API.
That said, our installation instructions and configuration instructions could use some review. I'm confident there's plenty to be updated.
A lot has been added over the past several releases, and I don't know that all the new menus are fully described. Even some screenshots would be nice to put in there for new users.
I'm definitely up on a comprehensive feature list and would love to help with that. Shawn has been doing work on something like this, but it's more a comparison of key features w/ other carts. I'd love to go through each part of the cart and itemize the features without being too annoying about every little thing. (ex: Awesome feature! You can view an order!!!)

Joined: 08/07/2007