By depositing silver nanoparticles (AgNPs) on the surface of aluminum nitride whiskers (AlNw), an AlNw-AgNPs heterogeneous structural filler was rationally designed from the perspective of interface engineering, which was further combined with nanofibrillated cellulose (NFC) to prepare anisotropic composite films by a facile vacuum-assited filtration method. Due to the synergistic effect of cross-linking AlNw and "thermal conducting micro-bridges" of AgNPs, the composite films exhibited an extraordinary in-plane thermal conductivity of 31.329 W m -1 K -1 , showing a promising application as thermal management materials.