<p>The investigation concerns carbon fiber–reinforced composites with a PTFE matrix, focusing on the effects of filler content and technological processing modes on mechanical, tribological, and supramolecular properties. An approach to composite fabrication is proposed, involving preliminary chemical functionalization of carbon fibers in an acidic medium (a mixture of sulfuric and hydrochloric acid solutions) to enhance interfacial adhesion. It is shown that functionalization increases tensile strength by up to 48 % (from 16.7 to 24.7 MPa) and Young’s modulus by up to 53 % (from 298 to 456 MPa), relative to composites with non-functionalized fibers. These increases correlate with enhanced interfacial adhesion and strengthening of the interphase layer. The tribological properties (coefficient of friction and mass loss) remain at their original levels, without any statistically significant degradation. Cold pressing with the application of ultrasonic vibration energy and low-frequency modulation produces a more uniform carbon fiber distribution, along with stabilization of the interfacial structure and an up to 32 % reduction in mass loss (from 0.65 mg/h to 0.49 mg/h). A correlation has been established between wear surface morphology and fabrication techniques. Comparative analysis of composites fabricated under different processing regimes confirms the efficacy of the proposed chemical functionalization in increasing stiffness and strength without deterioration of tribological properties.</p>