Calcium carbonate and carbon fiber surfaces were modified by use of a series of plasma polymers at different selected plasma conditions, and the effect of surface modification, mainly on the mechanical properties of composite systems prepared, was investigated. The matrices for the composite systems employed were polypropylene and epoxy, for the chalk and C fiber, respectively. Mechanical and thermal studies and scanning electron microscopy (SEM) pictures revealed that inclusion surfaces, being independent of their geometry and size, can be modified effectively by plasma. A polypropylene matrix with 30% modified chalk had better properties than composites with 10% unmodified chalk. Tensile strength and stress to failure values for single carbon fibers were found to be improved by plasma treatment. Surface-treated carbon fibers yielded at composites with better interlaminar shear strength and flexural strengths.