In this paper, the effects of different quenching temperatures on the microstructure and properties of Fe–4.0C–35.0Cr–0.5Si (wt.%) low-silicon hypereutectic high-chromium cast iron (LS-HHCCI) was investigated. The effect of quenching temperature on the microstructure of LS-HHCCI was analyzed by optical microscope, scanning electron microscope, and X-ray diffractometer. After quenching at different temperatures, the hardness and wear resistance of LS-HHCCI were tested by Rockwell hardness tester, microhardness tester, and wear testing machine. The results show that the microstructure of as-cast LS-HHCCI is mainly composed of austenite matrix and M7C3 carbides. After quenching, the austenite matrix is transformed into martensite, and M23C6 type secondary carbides are precipitated in the matrix. As the quenching temperature increased from 950 °C to 1100 °C, the eutectic carbides first appeared as fine needles, and then they gather and grow up, showing elongated or lumpy. The hardness and abrasion resistance first increase and then decrease, it reached peak values of 67.2 HRC at the temperature of 1050 °C, while the wear resistance is the best.