In this study, three kinds of metal chills such as SS400, AC4CH and brass, with different thicknesses of 40 ~ 80 mm, were applied for low pressure casting of Al-Si alloy to control cooling rate. The microstructural characteristics with increasing cooling rate were represented using factors including D1, D2, size of primary α phases and shape factor and size of eutectic Si. The tensile properties were investigated and additionally analyzed based on the microstructural characteristics. As the cooling rate increased, D1, D2, and sizes of primary α phases and eutectic Si apparently decreased and the shape factor of eutectic Si increased to over 0.8. The ultimate tensile strength (UTS) and yield strength (YS) increased with decreasing D1, D2, and size of primary α phases, while elongation increased with decreasing size of eutectic Si and concurrently increasing shape factor of eutectic Si. This indicated that the primary α phases and eutectic Si in Al-Si alloy were refined with increasing cooling rate, resulting in improvement of UTS and YS without sacrificing elongation. After the tensile test, preferential deformation of primary α phases was observed in the Al-Si alloy produced at higher cooling rates of more than 0.1 K/s.