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• α-MnSe Nanosheets are prepared via a facile hydrothermal method. • The effect of reaction time on electrochemical performance is investigated. • The α-MnSe electrode delivers a high capacity of 88.3 mAh g−1 at 1 A g−1. • The asymmetric supercapacitor exhibits a high energy density of 39.3 Wh kg−1. Transition metal selenides are regarded as emerging materials for energy storage devices because of their good electrical conductivity and electrochemical activity. Here, a binder-free ultrathin α-MnSe nanosheets electrode is prepared and the supercapacitor performance is comprehensively explored. Due to the increased active sites, enlarged contact area for electrolyte, as well as shorten ions diffusion pathway, the prepared electrode delivers high capacity of 88.3 mAh g−1 at 1 A g−1, good rate capability, and long-term durability (91% remain after 5000 cycles). Moreover, the asymmetric supercapacitor, fabricated by α-MnSe anode and active carbon cathode, displays a high energy density of 39.3 Wh kg−1 at a power density of 0.92 kW kg−1 and satisfying cycle performance. This study demonstrates that the binder-free α-MnSe electrode holds great promise for supercapacitor. [ABSTRACT FROM AUTHOR]