Four groups of granite aggregates with different mineral structures were investigated. They were formed into test plates with a flat surface and polished with the Aachen Rafeling Tester using quartz powder and quartz sand as the polishing agent respectively. At the end of each polishing stage, the friction coefficient of these plates was measured with the skid resistance tester (SRT) and the Wehner/Schulze test apparatus (PWS), which represent different contact conditions. By comparison of the different friction development in the course of polishing, the influence of mineral composition and crystal size on the polishing resistance and friction coefficient of the aggregates is determined. This new methodology can be applied to evaluate the long-term skid resistance of the aggregates for road engineering.