The nanoindentation behavior of DC magnetron sputtered 10 nm Cu and 10 nm Cu/2 nm Cr thin films deposited on Si (100) has been studied using a Hysitron nanomechanical system. X- ray diffraction and X-ray reflectivity were used to measure the film structure and film thickness, respectively. The grain size and orientation of Cu and Cu/Cr thin films were measured by TEM. Atomic force microscopy (AFM) was used to evaluate the surface morphology and roughness. At the same load, the nanoindentaion displacement of Cu/Cr is smaller than that for Cu, i.e., the 2nm thick Cr underlayer enhances the hardness of Cu. X-ray, TEM, and AFM results show that the grain size of Cu/Cr (< 15 nm) is actually larger than Cu (∼ 3 nm) indicating that the inverse Hall-Petch relationship may be operative.