widespread interest as promising candidate due to the advantages of high safety, good economy, and the intrinsic merits of Zn with low redox potential (−0.76 V vs standard hydrogen electrode), high theoretical capacity (820 mAh g −1 ), and energy density. [2][3][4][5][6][7][8] To fulfill the application potential of ZIBs, suitable cathode materials are highly critical to pair Zn anode. Hitherto, several types of cathode materials, such as manganese-based oxides, [9][10][11][12] vanadium-based oxides, [10,13] Prussian blue analogs, [14] and Quinone analogs, [15] have entered researchers' spotlight. The investigation yields consensus of MnO 2 as the most prevalent choice thanks to its good economy, low toxicity, high theoretical capacity, and working potential. [5,10,[16][17][18] However, the low electronic/ionic conductivity and non-negligible manganese dissolution of MnO 2 result in the inferior rate performance and fast capacity decay of MnO 2 -based cathodes, hindering the commercialization of ZIBs. [19][20][21] Great endeavors have been dedicated to improve the reaction kinetics and structural stability of MnO 2 -based cathodes in strategies of polymorphs regulation, [16,22] preintercalation, [18,[23][24][25][26][27][28] heteroatom doping, [29,30] compositing with conductive materials, [18,[31][32][33][34][35] and Mn 2+ additives of electrolyte. [9,36] All these strategies have been proven to effectively improve the electrochemical performance of MnO 2 -based cathodes in ZIBs to some extent. It is found that δ-MnO 2 (layered structure, typical with large interlayer spacing of ≈7 Å) could be more theoretically favorable for Zn 2+ insertion/extraction than their tunnel-structured counterparts (e.g., α-MnO 2 with 2 × 2 tunnels and β-MnO 2 with 1 × 1 tunnels). [5,16] Both preintercalation of guest species into MnO 2 and compositing MnO 2 with electrical conductive materials can improve its electrical conductivity, suppress manganese dissolution, and stabilize its structure. [18,21,25,28,34] Moreover, there are also considerable attempts to reveal the charge storage mechanism of aqueous mild Zn-MnO 2 batteries with the aim of further performance optimization. [5] Different energy storage mechanisms, such as Zn 2+ insertion/extraction, [35] H + /Zn 2+ coinsertion, [37] conversion reaction, [9] and dissolution/deposition, [38] have been proposed to explain certain ZIBs systems. With respect to the scientific progress, it is inferred that the significantly enhanced electrochemical performance of MnO 2 -based cathode are highly MnO 2 -based material is one of the most promising cathode candidates of aqueous zinc-ion batteries (ZIBs), but its commercialization is hindered by the sluggish reaction kinetics and poor structural stability. Herein, a hierarchical framework consisting of core-shell structured carbon nanotubes@K-birnessite-MnO 2 enwrapped by graphene/carbon black bicomponent networks (CNT@ KMO@GC) via a simple method for ZIBs is designed and developed. The hierarchical framework characterized with favorable K ...