A simple method for the preparation of rare earth ion-doped polymers, which display luminescence, is reported. For this purpose silicone–urea copolymers were doped with Nd(NO 3 ) 3 ·6H 2 O. Various structural and physicochemical properties of the resultant materials were investigated. FTIR studies indicated strong interaction of Nd 3+ ions with urea groups, but no interaction with siloxane backbone, which is expected. Absorption measurements in the visible and near infrared region were performed and the radiative decay rates and branching ratios for the meta-stable 4 F 3/2 level were determined by using Judd–Ofelt theory. The samples were also excited at 800nm and emission spectra were observed in the near infrared at 905, 1059, and 1331nm. In Nd 3+ doped silicone–urea systems the highest emission cross section at 1059nm was determined to be 60.7×10 −21 cm 2 . Spectroscopic parameters determined in this study suggest that Nd 3+ doped silicone–urea copolymers are promising candidates for the development of fiber lasers or amplifiers near 1.06 and 1.3μm.