Force‐Field Regulation Engineered Heterogeneous Graphene Micro‐Aerogels as Versatile Platforms for High‐Mass‐Loading Energy Storage

Abstract Achieving high areal energy density requires the development of advanced electrodes capable of maintaining excellent performance under high mass‐loading conditions. Herein, a novel force‐field regulation strategy has been proposed to fabricate graphene oxide/exfoliated graphene heterogeneous micro‐aerogels (GM) electrodes with precisely engineered channel structures and interconnected conductive frameworks. This innovative design effectively mitigates the limitations of conventional graphene aerogels (GA) and graphene films (EGF), such as prolonged ion transport paths and severe internal potential gradients, particularly under high mass‐loading. As a result, GM electrode, with a high mass loading of 20 mg cm ⁻² , demonstrates an outstanding capacitance of 2.53 F cm ⁻² at an operational time of 200 s, and maintains a superior 58.7% capacitance retention at a shorter time of 5 s, significantly outperforming its GA and EGF counterparts. Moreover, GM architecture can serve as a universal platform to host redox‐active faradic materials (e.g., PANI, MnO ₂ , and Co(OH) ₂ ), achieving exceptional areal capacitances up to 16.9 F cm ⁻² , demonstrating its versatility and scalability for energy storage applications. The underlying mechanisms driving the superior performance of GM electrodes are comprehensively elucidated through multiscale characterizations, electrochemical analyses, and finite element simulations, offering a robust framework for the design of next‐generation high‐mass‐loading energy storage systems.