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UV/ozone treated (UVO-treated) TaS2 and non-treated TaS2 nanosheets are introduced into organic photovoltaic cells (OPVs) as hole extraction layers (HEL) and electron extraction layers (EEL). TaS2 nanosheets are obtained via ultrasonic vibration and size-controlled by centrifugation. Atomic force microscopy (AFM) images reveal that the thickness and lateral size of TaS2 nanosheets are approximately 1 and 70 nm, indicating that uniform and ultrathin TaS2 nanosheets are obtained. The work function of TaS2 increases from 4.4 eV to 4.9–5.1 eV after applying UVO treatment by forming Ta2O5. In addition, the power conversion efficiencies of normal OPV with UVO-treated TaS2 and inverted OPV with TaS2 are 3.06 and 2.73%, which are higher than those of OPV without TaS2 (1.56% for normal OPV and 0.22% for inverted OPV). These results indicate that TaS2 is a promising material for HEL and EEL layers in …