where C is the specifi c capacitance, Δ V is the operating voltage range, and Q is the specifi c charge-storage capacity. For improving the specifi c energy, both the charge-storage capacity and operating potential window (OPW) of the pseudocapacitor electrodes should be maximized.First reported by Goodenough and coworkers, [ 13,14 ] MnO 2 has attracted substantial attention as a promising pseudocapacitor electrode material [ 15 ] because of its low cost, natural abundance, and environmental friendliness. The use of aqueous neutral electrolytes in MnO 2 -based pseudocapacitors, in particular, provides superior device safety compared with those requiring either organic electrolytes or strong acidic (such as for RuO 2 ) [ 16 ] aqueous electrolytes.Numerous studies have recently developed MnO 2 electrodes either in thin fi lm [17][18][19] or as composites with various materials, such as graphene, [ 20,21 ] porous carbon foam, [22][23][24] and SiC, [ 25 ] to increase the solid-electrolyte contact area and tailor the electrode architectures for enhanced capacity and power performances. [17][18][19][20][21][22][23][24][25] However, until now, the charge-storage capacity of MnO 2 -based pseudocapacitors has been limited to a small fraction of oneelectron transfer between Mn(IV) and Mn(III) ions per unit formula of MnO 2 ( e − /MnO 2 ) with an OPW of ≤1 V. [ 26 ] Only in rare cases of either extremely low oxide loading [ 22,27,28 ] or mixed valences, [ 21 ] the MnO 2 electrodes have been reported to afford a specifi c charge capacity close to 1 e − /MnO 2 . To exceed this charge-storage limit, new strategies that enable reversible electron transfer between Mn ions of lower valences are required, and this also means that the OPW must be extended to lower potentials.For an MnO 2 electrode in an aqueous electrolyte, the upper limit of its OPW is typically not related to the intrinsic properties of the oxide; however, it is limited by either water (solvent) or electrolyte anion (e.g., Cl − ) oxidation, [ 29 ] or current collector oxidation, [ 30 ] or the combination of both. For example, water oxidation causes oxygen bubbling, which may lead to active-layer loosening, and current collector oxidation causes an increase in the interfacial resistance between the active layer and the current collector. By contrast, the lower limit of the OPW of an MnO 2 electrode is closely related to the fundamental electrochemical Mn oxides are highly important electrode materials for aqueous electrochemical energy storage devices, including batteries and supercapacitors. Although MnO 2 is a promising pseudocapacitor material because of its outstanding rate and capacity performance, its electrochemical instability in aqueous electrolyte prevents its use at low electrochemical potential. Here, the possibility of stabilizing MnO 2 electrode using SiO 2 -confi ned nanostructure is demonstrated. Remarkably, an exceptionally good electrochemical stability under large negative polarization in aqueous (Li 2 SO 4 ) electrolyte, usually unattainable fo...