Sr co-doped Ce:LiCaAlF6 [Ce:Li(Ca,Sr)AlF6] crystals with various Ca/Sr ratios were grown by a micro-pulling-down (μ-PD) method and effects of Sr co-doping on crystal structure, chemical composition, optical and scintillation properties for Ce:LiCaAlF6 crystals were investigated as a neutron scintillator. High transparent Ce2%:Li(Ca,Sr)AlF6 crystals with 2% and 5% Sr contents were obtained while Ce2%:Li(Ca,Sr)AlF6 crystals with 10% and 20% Sr contents included milky parts in the crystals. a- and c-axis lengths of Ce:Li(Ca,Sr)AlF6 phase systematically increased with an increase of Sr content. In addition to the emission at 284 and 308nm from Ce3+ ion, emission peaks at 367nm appeared by Sr co-doping.