Hetero- and homoepitaxial Nd3+-doped LaF3 thin films have been grown by molecular beam epitaxy. Two different orientations of CaF2 substrates, (111) and (110), have been used for the heteroepitaxial structures. High-resolution emission and excitation spectra as well as the decay time of the emission have been measured. The spectroscopic measurements demonstrate that one Nd3+ site is present in the LaF3 layers grown on CaF2(111) substrates but two slightly different Nd3+ centers are resolved in the films on CaF2(110) substrates. One Nd3+ site has been found in the homoepitaxial sample. Slight differences are observed between the centers found in the LaF3 layers and the one observed in the Nd3+-doped LaF3 bulk crystal. For the homoepitaxial layer, the linewidths are similar to those of the bulk crystals, whereas for the heteroepitaxial layers, a broadening is observed.