Nd-doped LiNbO3 films have been prepared on (012) sapphire substrates by pulsed laser deposition. LiNbO3 phase is formed using Li rich targets, a 1.5×10−2 mbar oxygen pressure atmosphere, and heating the substrate to 520 °C. The crystallinity of 1-μm-thick films has been enhanced by postdeposition thermal treatments at 600 °C. The [Nd]/[Nb] concentration ratio in the film is equal to its value in the target; however, a limit for the Nd incorporation to the LiNbO3 phase has been found due to the preferential nucleation of Li deficient phases for [Nd]/[Nb]>0.1. The Nd photoluminescence of the films have been studied at 77 K exciting the F43/2 multiplet. The photoluminescence of congruent LiNbO3 single crystals is well reproduced in films prepared from targets with a [Li]/[Nb]=1.6 composition. Films prepared from targets with a [Li]/[Nb]=3 composition, additionally show an emission, with a main maximum at 1064 nm, the splitting of the F43/2 multiplet being 80 cm−1. The possible origin of the latter photoluminescence is discussed.