Here we demonstrated tantalum trisulfide (TaS3) nanowires as a new self-supported and flexible anode material for Li-ion batteries with high specific capacity and excellent electrochemical cycling. The TaS3 nanofibers were fabricated by a solid state reaction process, delivering a good reversible capacity of ∼400 mAhg(-1) after 100 cycles at 0.1C with only 0.1% decay per cycle compared with the initial charge capacity. Cycled at 10C, it displays a capacity as high as 60 mAh g(-1). The continuous and interconnected TaS3 nanowires not only enable fast access of electrons and ions but also grant the electrode with high mechanical flexibility.