Metal-organic frameworks (MOFs) possess significant potential in enhancing the interfacial performance of composites owing to their exceptional skeletal structures and substantial specific surface area. Herein, we prepared typical conductive MOFs (Ni-HHTP, HHTP = 2, 3, 6, 7, 10, 11-hexahydroxybenzene) at the interface by in situ synthesis using cellulose nanofibers (CNFs) assembled on the surface of carbon fibres (CFs) as precursors. CNFs can not only act as a smart cushion to promote stress release but also provide abundant oxygen-containing functional groups, such as hydroxyl and carboxyl groups, which can facilitate the growth of MOF on the surface of CFs. Furthermore, MOFs with porous structure and large specific surface area increase the interphase region for interfacial load transmission. The CF composites prepared using this strategy exhibited improvements in interlaminar shear strength (ILSS), interfacial shear strength (IFSS), flexural strength and flexural modulus by 57.9 %, 54.9 %, 35.1 % and 46.7 %, respectively. Additionally, the electrical conductivities of the composites in both thickness and in-plane directions were 1.04 × 10−4 S/cm and 7.3770 S/cm, respectively, which was attributed to the MOFs on the surface of the fibres facilitating the formation of good conductive channels between the fibres and resin. This study proposes an advanced interfacial modification approach to prepare CF composites with excellent mechanical and electrical conductivity properties.