Spatial changes of optical and mechanical properties of doped lithium niobate (LN, LiNbO3) single crystals are investigated. The crystals are doped with copper ions by thermal diffusion at elevated temperatures. LiNbO3 crystal absorption spectra are recorded in a direction perpendicular to the direction of diffusion. The concentrations of copper ions are calculated using the Smakula–Dexter formula. To determine a relation between changes of optical and mechanical properties, the hardness profiles of the doped crystals are investigated by the nanoindentation technique. Young's modulus and hardness are specified in accordance with the Oliver–Pharr method.