The AlFeCoNiCrTi high-entropy alloy (HEA) powders were prepared by high-energy ball milling. The ultrafine-grained WC–HEA and WC–Co-cemented carbides were fabricated through planetary ball milling and heat-pressure sintering. The microstructures and properties of the sintered alloys were compared using scanning electron microscope, X-ray diffraction, mechanical property testing and electrochemical testing. It has been shown that the AlFeCoNiCrTi HEA can be used as a binder for the ultrafine-grained WC-based cemented carbide. The WC–HEA-cemented carbide has better performances than the WC–Co-cemented carbide. The suitable contents of HEA can inhibit the WC grain growth and improve the mechanical properties and corrosion resistance of cemented carbides.