Carbon/carbon (C/C) composite materials are widely used in aerospace, the military and nuclear energy. The outstanding mechanical qualities of C/C composites mean that they are difficult to crush and recycle using traditional technology. The current recycling methods primarily involve stacking and landfill disposal. Therefore, achieving efficient and environmentally friendly recycling of carbon/carbon (C/C) composites is an urgent and challenging issue. In this work, we reported a simple high-value recycling approach for carbon–carbon frictional composite material (CFCM). The solid-state shear milling (S3M) technology is employed to achieve ultrafine milling of carbon matrices in carbon/carbon (C/C) composite materials while preserving carbon fibers. By this means, carbon fibers and the carbon matrix were mainly split, and the prepared composite powder had combined functionalities of conductivity, thermal conductivity, reinforcement, and wear resistance. The experimental results showed that the tensile strength of the material increased from 64.35 MPa to 72.79 MPa after being compounded with PA6, and the thermal conductivity increased from 0.211 W/mK to 0.611 W/mK. The friction coefficient was reduced from 0.51 to 0.36, a reduction of 25.4%, and the heat deflection temperature was increased from 47.2 °C to 108.2 °C. The S3M technique proposed in this work is an efficient, high-value, and scalable recycling strategy for CFCM, which can be used to produce value-added products and has great application prospects.