Because of the excellent thermal conduction, corrosion resistance, and tribological properties, copper-based friction materials (CBFMs) were widely used in airplanes, high-speed trains, and wind power generation. With operating speed continuously increasing, CBFMs are suffering more complicated and extreme working conditions, which would cause abnormal abrasion. This paper presents an experiment to investigate how the tribological behaviors of CBFMs are regulated by granulation technology. Samples were prepared by the method of granulation and cool-pressed sinter. The tribological properties of specimens with different granule sizes were studied. The results showed that granulation could improve the tribological properties of CBFMs. The friction coefficient (COF) increased first and then decreased with increasing granule size. Specimen fabricated with 5–8 mm granules obtained the lowest COF, which was reduced by 22.49% than that made of powders. Moreover, the wear rate decreased first and then increased as granule size increased. The wear rate of samples prepared by granules 3–5 mm was lower than that of all of the other samples. This is because the structured samples prepared by wet granulation can promote the formation of secondary plateaus, which are beneficial for enhancing tribological properties. This makes granulation a promising method for enhancing the tribological performances of CBFMs.