In this article, we report the results of the low-temperature chemical modification of a polyurethane (PU) surface using surface-wave excited N-2/H-2 plasma. Optical emission spectroscopy (OES) and double-probe measurement were performed to obtain optimum plasma properties. X-ray photoelectron spectroscopy (XPS) was employed to characterize the changes on the PU surface and to estimate the amount of introduced nitrogen-containing groups. The result shows that the largest amount of increase was obtained in the case of 90% N-2/(N-2 + H-2) plasma where the N/C ratio on the PU surface increased from 0.0128 before plasma treatment to 0.131 after plasma treatment.