Hardened ordinary Portland cement mortar pastes were prepared with different water / cement ratios within the range of 0.25 to 0.50 and cured for various time intervals up 28 days. At each hydration time the hardened specimens were, then, impregnated with different monomers; these are : castor oil (C.O), isocyanate and methyl methacrylate (MMA). Polymerization was carried out by subjecting the impregnated samples to different doses of γ-radiation where polyurethane (PU), polyurethane-methyl methacrylate copolymer were formed within the pore system. The influence of polymer impregnation of the various physico-mechanical characteristics of the resulting composites, namely, compressive strength, of the samples in connection with water cement ratio, radiation dose and curing period was discussed. Scanning electron microscopy (SEM) was employed to study the microstructural characteristics of the neat hardened OPC mortar pastes and their polymer-impregnated composites.