Bendable lithium secondary batteries have many limitations, including low electrochemical performances and poor mechanical flexibility. Here, we bendable pouch batteries are fabricated using LiFePO4/C as the active material and three-dimensional Nickel-Chromium alloy metal foam as the current collector of positive electrodes. The advantages of using the three-dimensional structured metal foam include a high surface area for the redox reaction, high electronic conductivity, and short diffusion length for the lithium ion. We demonstrate the use of bendable lithium secondary batteries with a high areal capacity of about 3.5mAhcm−2 at C-rate of 0.2, a high capacity retention rate in cycle life behavior, and a greatly low charge transfer resistance of around 6–8Ω. Moreover, our bendable pouch batteries can be repeatedly bent to radii of 12.5 and 2.5mm for several hundred times without fractures in the electrode and capacity fading.