Carbon fiber-reinforced polymers based on polystyrene matrix containing elastomer and carbon nanotubes (CNTs) were produced by compression molding. The effects of carbon fabric (CF) concentration and silane treatment on the morphology, mechanical, electrical, and shape memory properties of the multilayer composites were investigated. The SEM analyses showed that fibers of the silane-treated CFs were more homogeneously covered with the polymer layers than the untreated CFs. The tensile strength and modulus of the composites increased by 521% and 125%, respectively, with an increasing number of CF plies from one to five. Upon silane treatment, the tensile strength of the multilayer composite improved by 26%, and the tensile modulus decreased by 18.4%. Electrical conductivities of the composites were in the semiconductor region due to the presence of both CNTs and CFs. 100% shape recovery less than a minute recovery time was obtained for all the composites with electrically triggered bending test.