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Thermoset/thermoplast and gypsum copolymer composites were prepared as ureaformaldehyde (UF) copolymerized with acrylic acid monomer at various gamma radiation doses, where the latter monomer produced the greatest improvement in mold stability as cracks treatment, weight loss, hardness, and water absorption. This is due to water absorption showing an increase in water uptake for UF-gypsum composites containing high amounts of acrylic acid monomer copolymerized through the irradiation process, producing a hydrophilic mold able to retain water from evaporation and weight loss, thus obtaining an unshrinkable crackless mold. The influence of acrylic acid and the gamma irradiation process on water absorption, gelation time, weight loss, surface hardness, and compressive strength was studied. The results showed improvement of mechanical flexibility with a reduced sensitivity to cracks indicating the possibility of using these improved molds after mixing with gypsum in the field of construction as inner partition panels and tile seals.