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Ce 0.1, 0.5, 1.0, and 2.0 mol%-doped K2NaLuF6 crystals with 2 mm in diameter and 30-50 mm in length were grown by micro-pulling-down method. The photoluminescence spectra under ultraviolet excitation showed intense emission ascribed to 5d-4f transitions of Ce3+ replacing Lu3+ isolated octahedral site. In the radioluminescenced spectra under alpha-ray irradiation, the emission band is due to the transition from the lowest 5d excited state of Ce3+ to 2F5/2 ground state level is dominant. The light yields of Ce:K2NaLuF6 under 5.5-MeV alpha-ray excitation was estimated to be approximately 1.2 to 1.8% of those of BGO.