Designing novel efficient electrode materials with controlled hierarchical structure and composition for advanced supercapacitors remains a great challenge. Herein, a core-triple-shelled hierarchical GCNF/PANI/NCO nanostructure has been designed and fabricated by sequential growth of the conductive polyaniline (PANI) layers and nickel carbonate hydroxide (Ni₂(CO₃)(OH)₂) nanosheets on the graphene-coated electrospun carbon nanofibers (GCNF) via a facile wet-chemical strategy. Taking full advantage of the free-standing architecture of graphene-coated electrospun carbon nanofibers, high conductivity and flexibility of the PANI layers, and abundant active sites of Ni₂(CO₃)(OH)₂ nanosheets, the optimal GCNF/PANI/NCO (2 h) electrode exhibits a high specific capacitance of 1565F g⁻¹ at 1 A/g and enhanced rate capability, which are higher than those of the GCNF, GCNF/PANI, and GCNF/NCO (2 h) electrodes at the same situation, and also exceeds most of the reported nickel carbonate hydroxide-based electrodes in literature. The superior performance should be mainly ascribed to the collaborative contribution of each component. Moreover, a self-assembled GCNF/PANI/NCO//AC hybrid supercapacitor delivers a high energy density of 35.4 Wh kg⁻¹@750 W kg⁻¹ and a long cycle lifespan. This strategy enables the controllable synthesis of core-triple-shelled hierarchical materials applicable to advanced electrochemical applications.

为高级超级电容器设计具有受控层次结构和成分的新型高效电极材料仍然是一个巨大的挑战。在此，通过连续生长导电聚苯胺 (PANI) 层和氢氧化碳酸镍 (Ni ₂ (CO ₃ )(OH) ₂ ) 纳米片在其上设计和制造了核-三壳层级 GCNF/PANI/NCO 纳米结构通过简便的湿化学策略制备石墨烯涂层电纺碳纳米纤维 (GCNF)。充分利用石墨烯涂层电纺碳纳米纤维的独立结构、PANI层的高导电性和柔韧性以及丰富的Ni ₂ (CO ₃ )(OH) _{2活性位点}纳米片，最佳 GCNF/PANI/NCO (2 h) 电极在 1 A/g 时表现出 1565F g ^-1的高比电容和增强的倍率性能，高于 GCNF、GCNF/PANI 和 GCNF/ NCO(2 h)电极在相同情况下，也超过了文献中报道的大部分碳酸镍氢氧化物基电极。卓越的性能应主要归因于每个组件的协作贡献。此外，自组装的 GCNF/PANI/NCO//AC 混合超级电容器可提供 35.4 Wh kg ^-1 @750 W kg ^-1的高能量密度和较长的循环寿命。该策略能够实现适用于高级电化学应用的核-三壳层级材料的可控合成。