AbstractHigh-performance functional fibers play a critical role in various indispensable fields, including sensing, monitoring, and display. It is desirable yet challenging to develop conductive fibers with excellent mechanical properties for practical applications. Herein, inspired by the exquisite fascicle structure of skeletal muscle, we constructed a high-performance bacterial cellulose (BC)/carbon nanotube (CNT) conductive fiber through in situ biosynthesis and enhancement of structure and interaction. The biosynthesis strategy achieves the in situ entanglement of CNTs in the three-dimensional network of BC through the deposition of CNTs during the growth of BC. The structure enhancement through physical wet drawing and the interaction enhancement through chemical treatment facilitate orientation and bridging of components, respectively. Owing to the ingenious design, the obtained composite fibers integrate high strength (939 MPa), high stiffness (52.3 GPa), high fatigue resistance, and stable electrical performance, making them competitive for constructing fiber-based smart devices for practical applications.