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Organic semiconductors are generally featured with low structure order in solid‐state films, which leads to low charge‐transport mobility and strong charge recombination in their photovoltaic devices. In this work, a “polycrystal‐induced aggregation” strategy orders the polymer donor (PM6) and non‐fullerene acceptor (L8‐BO) molecules during solution casting with the assistance of PM6 polycrystals...