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Carbonitrides-modified silver phosphotungstate (CN-AgPW) photocatalysts were synthesized by self-assembly and solid-phase thermal polymerization. The microstructural and optical properties of the synthesized photocatalysts were systematically investigated, and the photocatalytic activity was evaluated by the degradation of Aflatoxin B1 (AFB1) under visible light (λ ≥ 420 nm) irradiation. The synthesis process, the interaction of compounds, and Z-scheme charge transfer path of the synthesized photocatalysts were investigated. The rate constants k of CN-AgPW-5 are 12.95 and 12.50 times higher than those of CN-390 and AgPW-390, respectively. This study provides a new strategy for the synthesis and enhancement of photocatalytic efficiency of insoluble polyoxometalate photocatalysts.