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Not having done this, but having experience with great stuff in molds. I would say go slow with small amounts. Multiple layers. Also get yourself a spray bottle. Apply your layer then spray it with water. This will make the great stuff expand fully in minutes. Considering that this is a hands on operation you want the speed.

Alternatively you do know that you can pickup stryofoam heads at beauty shops for around $4 each? Might be more expensive solution, but your masks wont be stuck and you get that hole in the bottom for easy mounting.

Anyhow, if you do end up doing this, let me know! Would be interested to see how it goes.
 
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