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In semiconductor-mediated photocatalysis, the optical property of semiconductors is a key parameter and closely related to the conversion efficiency of solar energy. However, endeavors in achieving a wide spectral response of semiconductors are still limited in impurity incorporation or using other assistants. Here, we report on a structure-distortion-induced extension in the optical absorption of conjugated polymer semiconductors without relying on any extra species, by taking a typical example of two-dimensional graphitic carbon nitride (g-C₃N₄) nanosheets. Experimental and theoretical calculation results both identified the close relationship between the band structure and the structural distortion and the amount of the layers, while keeping in-plane fundamental units intact and the connecting mode invariable during the peeling process. Photocatalytic activity was evaluated toward hydrogen evolution over …