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Highlights The mechanical strength of polylactic acid (PLA) can be improved by carbon fiber (CF) compositing to expand its application in tissue engineering scaffolds. However, the mechanical strength of CF‐reinforced polylactic acid (CFRPLA) composites is compromised due to weak interfacial interaction resulting from the chemically inert surface of CF. In the article, carbon nanotube (CNT) with poly(diallyldimethylammonium chloride) (PDDA) as a coupling agent was covered on CF to improve the chemical activity and roughness of the surface of CF, and then the as‐prepared CF‐PCNT were further incorporated into PLA via melt compounding. The yield strength, modulus, and thermal conductivity of PLA/CF‐PCNT were 14.09%, 7.65%, and 5.24% higher than those of PLA/CF, respectively, and the volume resistivity was 99.74% lower at a 10 wt% loading. The enhancement for the mechanical properties of PLA/CF‐PCNT composites could be ascribed to the mechanical locking, hydrogen bonds and covalent bonds between CF and matrix through the interface modulation of CNT and PDDA. This facile and non‐destructive method offers a novel strategy for the modification of CF fillers. CF was modified by PDDA and CNT through a facile and non‐destructive method. The active functional groups and roughness on the surface of CF were increased. The surfaces of CFs were characterized by FT‐IR, Raman spectra, XPS and SEM. The interface was improved by mechanical locking, covalent, and hydrogen bonds. The mechanical strength, electrical and thermal conductivity of composites were improved. [ABSTRACT FROM AUTHOR]