This paper reports on an investigation of contact damage induced in molds and substrate materials used in micro- and nanoimprint lithography. Silicon, polydimethylsiloxane (PDMS), glass, and silicon carbide were studied. A finite element analysis using ABAQUS software was conducted to investigate the stress induced in mold and substrate materials when they come in contact with each other at a uniaxial pressure of 1 MPa. A spherical indentation experiment was conducted for a model study for various indentation loads and numbers of contact cycles. We examined the contact damage during the spherical indentation. Indentation stress-strain curves, surface views of contact damage, and mechanical properties were characterized for the mold and substrate materials.