Summary Polydopamine (PDA) films were irradiated by an electron beam linear accelerator at different irradiation doses ranging from 10 to 150 kGy. The irradiated samples were characterized by Fourier transform infrared spectrometry, UV‐Vis, scanning electron microscopy, atomic force microscope, X‐ray diffraction, cyclic voltammetry, electrochemical impedance spectroscopy, and thermogravimetric analysis. Changes in surface morphology, chemical structure, contact angle, frontier orbitals, and bandgap were analyzed. PDA films modified by electron beam irradiation were used in the interface design and control of polymer solar cells. Devices with the structures of ITO/ZnO/PTB7:PC71BM/MoO3/Al and ITO/PDA‐ZnO/PTB7:PC71BM/MoO3/Al were fabricated. The solar cells with a 100‐kGy electron beam‐irradiated PDA film‐modified ZnO electron transport layer had a significantly improved short circuit current density, and its efficiency reached a maximum value. The short circuit current density and power conversion efficiency reached 13.70 mA/cm2 and 3.82%, respectively. Electron beam irradiation is an effective method to modify PDA, which can be used as an interface modifier in polymer solar cells.

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