Two-dimensional (2D) crystalline porous materials with designable structures and high surface areas are currently a hot research topic in the field of proton- and electron-conducting materials, which provide great opportunities to orderly accommodate carriers in available spaces and to accurately understand the conducting path. The 2D dual-conductive inorganic framework [Co(H₂O)₆]₂{[Co(H₂O)₄]₄[WZn₃(H₂O)₂(ZnW₉O₃₄)₂]}·8H₂O (Co₆Zn₅W₁₉) is synthesized by combining [WZn₃(H₂O)₂(ZnW₉O₃₄)₂]^12- (Zn₅W₁₉) and a Co(II) ion via a hydrothermal method. Due to the presence of a consecutive H-bonding network, electrostatic interactions, and packing effects between the framework and guest molecules, Co₆Zn₅W₁₉ displays a high proton conductivity (3.55 × 10^-4 S cm^-1 under 98% RH and 358 K) by a synergistic effect of the combined components. Additionally, a photoactuated electron injection into the semiconducting materials is an important strategy for switching electronic conductivity, because it can efficiently reduce the frameworks without destroying the crystallinity. I-V curves of a tablet of Co₆Zn₅W₁₉ in the reduced and oxidized states yield conductivities of 1.26 × 10^-6 and 5 × 10^-8 S cm^-1, respectively. Moreover, Co₆Zn₅W₁₉ is also successfully applied in the photocatalytic reduction of the toxic Cr(VI) metal ion by utilizing its excellent electronic storage capacity and Baeyer-Villiger (BV) oxidation in a molecular oxygen/aldehyde system.

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