摘要： Through regulating the pH values, a series of iodo-argentate/cuprate hybrids, [Me3(4-TPT)]4[Ag6I18] (1, Me3(4-TPT) = N,N’,N’’-trimethyl-2,4,6-tris(4-pyridyl)-1,3,5-triazine), [Me3(4-TPT)][M5I8] (M=Ag/2, Cu/2a), [Me3(3-TPT)][M5I8] (Me3(3-TPT) = N,N’,N’’-trimethyl-2,4,6-tris(3-pyridyl)-1,3,5-triazine, M=Ag/3, Cu/4), exhibit adjustable structural variations with different dimensional structures, have been obtained under solvothermal conditions. They are directed by two types of in situ N-alkylation TPT-derivatives (Me3(4-TPT) for 1/2/2a and Me3(3-TPT) for 3/4) and represent the isolated units (1), 1-D polymeric chain (4), 2-D layered structures (2/2a, 3) based on diverse metal iodide clusters. These compounds possess reducing band gaps comparing with the bulk β-AgI and CuI and belong to potential semiconductor materials. Iodocuprates feature highly efficient photocatalytic activity in sunlight-induced degradation of organic dyes. The detailed study on the possible photocatalytic mechanism, including the radical trapping tests and theoretical calculations, reveals that the N-alkylation TPT moieties contribute to the narrow semiconducting behavior and effectively inhibit the recombination of photogenerated electron–hole pairs, which result in an excellent visible-light induced photocatalytic performance.