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Great stuff is really sticky stuff when wet so i would guess no but i am by no means a pro like the rest of the people on here.
 

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Grim, you can use greatstuff, but it is a bit unpredictable to make castings with. Put a thin layer of vaseline in your mold as a release agent, and allow several days for it to cure 100%. When I started casting, I used greatstuff for quite a while with fairly decent results

...HOWEVER....if you have access to 2 part urethane foam (many places to purchase on the net) you will not be dissapointed... it is a much better product for casting , and if you can swing the initial cost your skulls end up being less expensive than using greatstuff.
 

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I have one of Daves skulls from the 2 part urethane and they are relly nice. Ive tried to mold other things with great stuff and it was a disaster.
 
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