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[Display omitted] • The ultrathin RhIr NSs/NF was prepared by a simple and mild one-pot aqueous strategy at room temperature. • The unique sheet-like architectures provided large ECSA and exposed high-density active sites. • The self-supported RhIr NSs/NF had excellent HER activity and stability for the HER over a wide pH range. The development of low-cost and high-efficiency electrocatalysts is very important for electrocatalytic hydrogen evolution reaction (HER) in water splitting system. Herein, ultrathin rhodium-iridium nanosheets were facilely in-situ grown on nickel foam (RhIr NSs/NF) by a one-pot aqueous strategy at room temperature. The sheet-like structures with the film thickness of 78 nm were identified by scanning electron microscopy and transmission electron microscopy. The catalyst showed greatly high HER features in both 1.0 M KOH and 0.5 M H 2 SO 4 with the overpotentials of 15 and 14 mV to achieve 10 mA cm−2, respectively, surpassing most Pt-free catalysts. Also, the RhIr NSs/NF exhibited amazing catalytic stability during the long-term operation. This study offers a facile and rational pathway for design and synthesis of advanced HER electrocatalysts for energy conversion devices. [ABSTRACT FROM AUTHOR]