| Summary: | The advantage of low resistivity and inactive binders makes binder-free electrode an excellent candidate for high-performance energy devices. A simple hydrothermal method was used to fabricate M<sub>11</sub>(HPO<sub>3</sub>)<sub>8</sub>(OH)<sub>6</sub> (M: Ni and Co) (MHP) arrays combined with activated carbon fabric (ACF) without binder. The structures of MHP can be easily tuned from bouquets to nano-sheets by the concentration of NaH<sub>2</sub>PO<sub>2</sub>. The MHP/ACF composite materials with different structures showed the typical battery-type characteristic of anodic electrodes. In a three-electrode cell configuration, the MHP nano-sheet arrays/ACF composite has a higher capacity, of 1254 F/g, at a scan rate of 10 mA/cm<sup>2</sup> and shows better cycling stability: 84.3% remaining specific capacity after 1000 cycles of charge-discharge measurement. The composite is highly flexible, with almost the same electrochemical performance under stretching mode. The MHP/ACF composite@ACF hybrid supercapacitor can deliver the highest energy density, of 34.1 Wh·kg<sup>−</sup><sup>1</sup>, and a power density of 722 W·kg<sup>−</sup><sup>1</sup> at 1 A·g<sup>−</sup><sup>1</sup>. As indicated by the results, MHP/ACF composite materials are excellent binder-free electrodes, candidates for flexible high-performance hybrid super-capacitor devices.
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