Although polymer solar cells (PSCs) have many advantages, they have obtained great progress in the two decades, the low charge carrier mobility still restricts performance progress of PSCs. Two-dimensional (2D) Bi-based semiconductor nanomaterial (Bi2OS2) can be a potential material for improving the charge carrier mobility in the active layer of PSCs, because it exhibits a high carrier mobility, suitable band gap, wide absorption range, and good stability. In this work, we synthesize the 2D Bi2OS2 nanomaterial and incorporate it into active layer of PSCs as a third component for the first time. By introduction 1 wt% 2D Bi2OS2 nanomaterial into the PSCs, the power conversion efficiency (PCE) of PSCs can be obviously improved by more than 17% comparison with binary PSCs (from 10.51% to 12.31%). The enhancement of PCE is mainly due to the improving of charge transport, surface morphology, and crystallization of active layer. It is worth noting that the 2D Bi2OS2 play the role of the heterogeneous nucleation in the active layer, resulting in the enhanced crystallization of PBDB-T and ITIC. These results not only provide a way to improve the performance of PSCs, but also show that the 2D Bi2OS2 nanomaterial has great potential application in the PSCs.