“…Semiconductor-based photocatalysts have attracted significant attention owing to their direct and efficient production of hydrogen via the conversion of solar energy into storable chemical energy. [1][2][3][4] Compared with inorganic semiconductor materials, [5][6][7][8][9] organic semiconductors, [10][11][12][13][14] in particular, linear conjugated polymers (LCPs) with the advantage of low cost, metal-free, structural diversity, solution processibility, and delocalized 𝜋 system, are more intriguing for solar-to-hydrogen (STH) photocatalytic applications. [15][16][17] However, owing to the inefficient molecular structure regulation of the building blocks on conjugated polymer backbones, they always show low crystallinity and intrinsic electron trap-site density, [18][19][20] leading to poor photocatalytic performance.…”