Abstract: With the rapid development of electronic products, electric vehicles and smart grids, lithium-ion batteries (LIBs) are required to not only possess superior lithium storage performance, but also be low-cost, abundant resources, and foremost sustainable. Based on the advantages of carbon anode materials, a smart strategy to convert the used bamboo chopsticks into uniform carbon fibers (CFs) by using the abundant natural fibers in chopsticks after a simple hydrothermal treatment was proposed. Compared with graphite electrodes, bamboo-based CFs exhibits excellent electrochemical performance as a sustainable anode of LIBs. Moreover, the lithium storage performance of CFs can be further upgraded by integrating nanostructured molybdenum disulfide (MoS₂) onto their surface by hydrothermal method to form the CFs/MoS₂ composite with a core-shell structure. The electro-chemical results show that the CFs electrode cycled 500 times at a current density of 200 mA/g, has a specific discharge capacity of 381.1 mA·h/g. And the CFs/MoS₂ composite electrode still maintains a specific discharge capacity of 843 mA·h/g at a high current density of 1000 mA/g for 1000 cycles.