Jayasinghe, RRamos, MNand, ARamezani, M2025-06-262025-06-262025-05-28Macromolecular Materials and Engineering, ISSN: 1438-7492 (Print); 1439-2054 (Online), Wiley. doi: 10.1002/mame.2025000881438-74921439-2054http://hdl.handle.net/10292/19391This investigation elucidates a novel methodology for augmenting the tribological and mechanical attributes of epoxy composites via selective functionalization of multi-walled carbon nanotubes (MWCNTs). The study optimizes wear mechanisms and friction-induced graphitization by incorporating pristine (P-MWCNTs), carboxyl-functionalized (COOH-MWCNTs), amine-functionalized (NH₂-MWCNTs), and silane-modified MWCNTs. Composites were characterized for tensile strength, compressive strength, surface hardness, coefficient of friction (COF), and specific wear rate (SWR). Incorporation of 0.3 wt.% COOH-MWCNTs yielded optimal performance, reducing SWR by 82% (0.07 × 10⁻⁶ mm³ N⁻¹·m⁻¹ at 8 Hz) and COF by 32% (0.37 at 10 N) relative to neat epoxy (SWR: 0.50 × 10⁻⁶ mm³ N⁻¹·m⁻¹, COF: 0.66 at 15 N). Enhanced dispersion, interfacial adhesion, and tribofilm formation account for superior tensile strength (≈90 MPa) and hardness (≈88 Shore D). X-ray diffraction and transmission electron microscopy validated friction-induced graphitization and partial structural degradation above 10 N. Applications encompass self-lubricating bushings, protective coatings, and wear-resistant surfaces for automotive and industrial components. Future investigations should target enhanced compressive strength and load-bearing capacity.© 2025 The Author(s). Macromolecular Materials and Engineering published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.http://creativecommons.org/licenses/by/4.0/40 Engineering4016 Materials Engineering03 Chemical Sciences09 EngineeringPolymers34 Chemical sciences40 EngineeringJournal ArticleOpenAccess10.1002/mame.202500088