I've been working my way through this. It's fascinating and accessible, and, at least when the lectures were recorded a few years ago, full of open problems.
The man is seriously goofy too. He made videos about demonstrating equivalence classes by rolling his father into a cube. And that was for an honorary title in some math circle.
Recently I bought the book "Geometric Folding Algorithms: Linkages, Origami, Polyhedra" he co-authored. That was the most expensive book I ever bought.
This page has a better version with more resources (lectures, classes, synced slides and notes): http://courses.csail.mit.edu/6.849/fall12/lectures/