Casting and mold polymerization processes were investigated by means of γ‐irradiation of methyl methacrylate prepolymer systems containing some quantity of polyfunctional monomers. Some physical properties, such as supercooling tendency and temperature dependence of viscosity and relaxation time in fluid prepolymers, were measured and related to cast polymerization at low temperatures. It was found that free‐state casting with no frame or mold was possible using viscous states of prepolymer in the supercooled state. Furthermore, efficient mold polymerization using soft gel prepolymer was studied. That is, plastic soft gel prepolymer was prepared conveniently by irradiation of fluid prepolymer, then molded into spherical or nonspherical curved surface shapes, and curved by reirradiation. Polymerization and gelation behavior of soft gel prepolymer and penetration degree of prepolymer as a measure of plasticity of gel were studied in relation to prepolymer composition and irradiation condition. Copyright © 1979 John Wiley & Sons, Inc.