High‐performance and integrated power sources are critical to the practical application of wearable sensors, enabling monitoring of physical signs in real time. However, realizing both good battery performance and portability for batteries is still a challenge to such integration application. Herein, a novel cathode material of flexible zinc–air battery is developed, i.e., NiFe‐based metal–organic frameworks nanoflakes assembled on the carbon frameworks with nitrogen‐heteroatom dopant (NiFe NF/NCFs). Benefiting from the unique interfacial interaction of 2D materials, as well as the rational integration of multifunctional electrocatalytic components in a flexible and compressible skeleton, the prepared NiFe NF/NCFs exhibits excellent activities for oxygen evolution/reduction reactions. Moreover, it achieves high peak power density (107.2 mW cm−2) and specific capacity (814.2 mAh g−1) when served as the cathode of zinc–air batteries. Importantly, serving as both battery cathode and sensing unit, a strain sensor–battery integration device is also demonstrated based on the NiFe NF/NCFs, which displays a favorable strain sensitivity toward detecting human motions. This work provides a new pathway to the development of energy storage device for flexible electronics.