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Because there is an overlap of the 5d-4f emission transition of Tm3+ and absorption transition of Nd3+, an energy transfer between Nd3+ and Tm3+ in LaF3 was supposed to enhance the efficiency of the previously studied Nd:LaF3 scintillation material. In this study, 0.1% and 1%Tm, Nd, and Tm, Nd codoped LaF3 single crystals scintillators were developed using micro-pulling down method (μ-PD), and their optical properties in the vacuum ultraviolet (VUV) region were evaluated. Tm3+ codopant did not show positive contribution to VUV emission, but energy transfer between Nd3+ and Tm3+ cannot be excluded, although the photoluminescence spectra point just to a competition for energy between the two ions. Gamma-ray response was also measured using the pulse-height distribution measurement.