Aqueous zinc-ion batteries (AZIBs) with MnO2 cathodes have promising application prospects, however, their performance is hindered by their low efficiency and insufficient life. By leveraging the nanomicellar properties of cetyltrimethylammonium bromide (CTAB), a hierarchical δ-MnO2 with 2D/3D structure was directionally grown on a modified carbon cloth (CC) collector for realizing high-mass-loading AZIBs. Experimental results reveal that the synergistic effects of micro/nano hierarchically structured MnO2–CC heterointerfaces in accelerating electron migration and transfer rate of Zn2+/H+. Functioning as a conductive skeleton and flexible substrate, CC efficiently improves the reaction kinetics and buffers the interfacial stress resulting from the structural evolution of MnO2 during the long-term electrode reaction. This phenomenon is investigated using advanced characterisation techniques, including X-ray absorption fine structure spectroscopy, Kelvin probe force microscopy, and theoretical simulations. The fabricated electrode exhibits superior electrochemical properties, such as high capacity (409.6 mAh g–1 at 0.1 A g–1) and reliable cycling performance (with 86.6% capacity retention after 2000 cycles at 1.0 A g–1). Even at a high mass loading of 6.0 mg cm–2, the battery retains 81.8% of its original capacity after 1300 cycles. The proposed interface engineering strategy provides valuable insights into realising high-loading and long-life AZIBs.

This article is Open Access

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