2D Laminated Hybrid Architectures Based on Graphene/Mesoporous Polyaniline for High‐Performance Supercapacitor Electrode

ABSTRACT Graphene has emerged as a highly promising candidate for high‐performance supercapacitor electrodes. Its atomically‐thin 2D structure and exceptional physical properties provide an ideal foundational platform for designing hybrid nanomaterials, which are pivotal for advancing electrochemical performance metrics. However, the practical use of these graphene‐based hybrids faces key challenges, including the degradation of electronic properties due to defects introduced during synthesis, and the insufficient control over the loading and distribution of pseudocapacitive components, which compromises their synergistic potential. To address these fundamental issues, we developed a novel 2D laminated hybrid architecture by using electrochemically exfoliated graphene (EG) and mesoporous polyaniline (PANI) nanosheets, synergistically combining electrical double‐layer capacitance and pseudocapacitance. A high‐shear mixing technique ensures uniform nanoscale blending at various ratios while preventing graphene restacking. Strong interfacial interactions confirm the formation of a laminated hybrid architecture, leading to an optimized microstructure with significantly enhanced charge storage characteristics. The hybrid electrode achieves a remarkable volumetric capacitance of 424.58 F/cm ³ and superior rate capability. Our work provides a rational design approach for the construction of graphene‐based 2D laminated hybrid architecture, advancing next‐generation energy storage technologies.