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In this paper, nanoporous copper (NPC) was prepared by dealloying ZrCuAl metallic glass ribbons with HF acid solutions. The effect of dealloying time on the porous structures and thickness of the obtained NPC films was investigated. It was found that the ligament sizes of the NPC could be tuned in a range from 20 to 300 nm, and the thicknesses of the NPC films from 3.1 to 14.4 μm, with properly selected dealloying times. Furthermore, nanoporous composites made of NPC and nanoporous Cu2O were prepared by oxidizing the NPC with ethanol. The nanoporous composite electrodes exhibited superior charge-discharge performance and would have broad potential applications in flexible high-performance energy storage devices.