Engineered living materials (ELMs) are an emerging class of materials that integrate living biological entities such as engineered bacteria with functional soft materials. The incorporation of functional bacteria enables unique capabilities such as self-regenerative, self-healing, biosensing, and molecular computing. Despite the recent progress in ELMs, the creation of ELMs and their derived materials with high physical properties such as mechanical strength or thermal conductivity is still very challenging. Here, I will present our recent research progress on the creation of hierarchical biocomposites with exceptional thermal conductivity based on synergistic microbial biosynthesis. Two types of engineered bacteria with the ability to generate bionanofibers and metal oxide nanoparticles were synergistically utilized together with fluorographene to create hierarchical biocomposites with highly ordered internal structure and high thermal conductivity. The in-plane thermal conductivity of such biocomposites is as high as 30 W/mK and can be widely tuned by adjusting the biosynthesis procedure and the content of 2D nanofillers. The biocomposites also show high flexibility, mechanical strength, and electrical resistance. Our approach of creating biocomposites with high thermal conductivity from ELMs has significant advantages in terms of sustainability, internal structure control, and low energy cost and carbon emission compared with conventional thermal interface materials.