Natural polymer hydrogels are considered to be excellent candidates for eco-friendly flexible devices. However, the defects of low strength and poor toughness result in their being easily damaged. Here, strong gelatin-based hydrogels enhanced by hydrophobic aggregation were prepared using salting-out treatment. Moreover, the cellulose nanofiber (CNF) with large aspect ratio further improved the mechanical strength relying on the intertwining effect. The optimized strong hybrid gelatin/CNF hydrogel achieved 0.73 MPa of breaking strength and 250% of elongation at break, 405 and 8.3 times that of the original hydrogel, respectively. Notably, the gelatin/CNF hydrogel exhibited satisfactory conductivity and excellent linear sensing behavior, allowing it to monitor human motions accurately. Besides, this robust gelatin-based hydrogel could be used as supercapacitor electrolyte and showed desirable rate capability and good cycling stability. This work implies a bright future for the application of gelatin-based hydrogel in the field of environmentally friendly energy storage devices and sensors.

天然聚合物水凝胶被认为是环保柔性设备的优秀候选者。然而，强度低、韧性差的缺陷导致其容易损坏。在这里，使用盐析处理制备了通过疏水聚集增强的强明胶基水凝胶。此外，大纵横比的纤维素纳米纤维（CNF）依靠缠绕效应进一步提高了机械强度。优化后的强混合明胶/CNF水凝胶的断裂强度为0.73 MPa，断裂伸长率为250%，分别是原始水凝胶的405倍和8.3倍。值得注意的是，明胶/CNF水凝胶表现出令人满意的导电性和出色的线性传感行为，使其能够准确监测人体运动。除了，这种坚固的基于明胶的水凝胶可用作超级电容器电解质，并显示出理想的倍率性能和良好的循环稳定性。这项工作预示着明胶基水凝胶在环保储能装置和传感器领域的应用前景广阔。