Design and fabrication of flexible free-standing electrode is crucial in the rapid advances of durable/flexible electronic devices. Herein, a unique functional electrode made of hierarchical MoS2 nanosheets anchored on electrospun poly (vinylidene difluoride) based fibrous membrane, has been developed through a facile hydrothermal method. When assessed as membrane electrodes in lithium-ion batteries, the as-prepared anodes exhibit a high capacity (854 mA h g(-1) at 0.5 A g(-1) and 513 mA h g(-1 )after 200 cycles at 2 A g(-1)), excellent rate capability, and long cycling life durability (332 mA h g(-1) at 5 A g(-1) after 1000 cycles). Grafting MoS 2 nanosheets onto 3D electrospun framework not only shortens the Li(+)diffusion path and increases their valid and accostable active surface area, but also invests it with flexible feature. Full membrane cells containing LiNi(0.5)Co(0.3)Mn(0.2)O(2 )cethode also gain excellent capacity performance, distinctive cycling tolerance and a high capacity preservation of 92% after 250 cycles even in the 90 degrees bending position, which are among those of the so far reported best-performing flexible lithium-ion batteries. This research offers a promising avenue for the exploitation of high-powered flexible lithium-ion batteries and other rechargeable batteries.