I've tried casting a bit, but not two part molds, only simple things like seats, wheels, prop blades. Just remember you'll need RTV rubber for the molds, two part casting resin, and mold release agent for making the two part molds. And lots of legos! Legos make great bases and walls for making your molds, and you can use them to make alignment marks for two part molds.
One technique I'd like to try is vacuum molding. If you reduce the pressure while casting, it can lead to fewer air bubbles trapped in the castings.