Nd 3+ -doped LaF3 heteroepitaxial waveguide films on two oriented CaF2 substrates were grown by the molecular-beam-epitaxy method. The spectroscopic properties of Nd3+ in the epitaxial films have been studied by using a tunable Ti:sapphire laser. Efficient IR emissions have been detected at 1.06, 0.86, and 1.32 nm ranges. The influences of substrate orientation, Nd3+ concentration, and temperature on the luminescence properties were investigated. By using a prism-coupling technique, waveguided luminescence has been measured at room temperature. Furthermore, laser emission at 1.06 μm was obtained at room temperature with a 790 nm laser pump.