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Exfoliated TaWO6 nanosheet was obtained by delaminating a layered compound HTaWO6 and assembled into multilayer films by a layer-by-layer deposition technology.The investigation on the photoelectrocatalytic degradation of Rhodamine B with the TaWO6 nanosheet electrodes exhibited that both the oxygen anionic radicals and the dye cationic radical are essential to mineralize the dye under visible-light-driven photocatalytic conditions.