Efficiency of bioelectrochemical systems (BESs) is generally limited by the performance of bioanode, resulted from the nature of microbial electron transfer and the character of the anode substrate. In the present study, a 3D structured anode material is fabricated using a towel as precursor through high-temperature carbonization. The 3D electrode is resulted from freely standing threads, twisted by fibers with diameter at micrometer scale, on a woven textile substrate. The open structure provides easy accesses for microbial to attach on the fiber surface. Furthermore, the prepared materials possess a high capacitive character which is beneficial for electron storage and contributes to the performance of bioanode. When tested in BESs, the prepared material achieves a current density of 0.80 ± 0.06 mA cm−2, larger than conventional anodes, e.g. graphite felt (0.55 ± 0.01 mA cm−2), carbon cloth (0.06 ± 0.01 mA cm−2), and carbon mesh (0.02 ± 0.00 mA cm−2). The present study provides a novel 3D anode substrate that can effectively promote the performance of BESs.