catalyst surface to form the final product, which seriously hinders the progress of the reaction. [3,4] Although researchers have made significant progress in the design of catalysts, a large cell voltage is still needed to drive this process. Therefore, it is still highly desirable to design high-efficiency water-splitting electrocatalysts. Recently, ruthenium (Ru) has attracted special attention for water-splitting catalysis since its inherently excellent activity and far lower price than platinum (Pt) and iridium (Ir). [5-9] To date, various strategies have been applied to enhance the activity of the Ru-based catalysts, including turning the crystal phase, doping electrocatalysts with hetero atoms, alloying Ru with the transition metals, and so on forth. [7,10,11] In principle, since the electrocatalysis is usually carried out on the surface of a catalyst, controlling the surface structure of the catalyst is a more straightforward way to improve the catalytic performance. The high-index crystal facets have more coordination unsaturated atoms and more active sites, which is believed to be more active. [12-14] Nevertheless, there were fewer reports on controlling the Ru-based catalysts with high-index facets. To this end, the fine control of Ru-based catalysts is of great significance in both practical application and fundamental research. Shape control has realized huge success for developing efficient Pd/Ptbased nanocatalysts, but the control of Ru-based nanocrystals remains a formidable challenge due to the inherent anisotropy in hexagonal closedpacked nanocrystals. Herein, a class of unique RuCo nanoscrews (NSs) for water electrosplitting is successfully synthesized with rough surfaces and the exposure of steps and edges. Those high-index faceted RuCo NSs show superior performance for overall water electrosplitting, where a low cell voltage of 1.524 V (@ 10 mA cm −2) and excellent stability for more than 20 h (@ 10 mA cm −2) for overall water electrosplitting in 1 m KOH is achieved. The enhanced performance of RuCo NSs is due to the optimization of the binding energy with the intermediate species and the reduced energy barrier of water dissociation. Density functional theory calculations reveal that the RuCo NS structure intrinsically endows various ridges and edges, which create low coordinated Ru-and Co-sites. These active Ru-and Co-sites present high efficiencies in electronic exchange and transfer between adsorbing O species and nearby lattice sites, guaranteeing the high H 2 Osplitting activities. This present work opens up a new strategy for creating high-performance electrocatalysts for water splitting.