What is it you're trying to accomplish? Are you wanting to smooth it out, or are you just wanting to make it more rigid? If you're trying to smooth it out, bondo is your best (cheapest and most readily available) option. If all you're wanting to do is make it more rigid, coat it 3-4 times in fiberglass resin (available at Lowes, Home Depot, any auto parts store, even Walmart has it). The pep guys will tell tell you resin is the way to go. The basic process goes like this...
-create your base model, ie your bio helmet
-give it a good coat inside and out to stiffen it up
-use fiberglass cloth inside to make it as rigid as possible
- add bondo (or some other sort of body filler) on the outside of the mask to shape and smooth it.
-finish with paint, or whatever you have in mind.
My advice is to do a google search for 'how to finish pepakura'. There's tons and tons and tons of info and video already out there that will guide you step by step through the process.
Brian