Abstract: | Uniform Ni3C nanodots dispersed in ultrathin N‐doped carbon nanosheets were successfully prepared by carburization of the two dimensional (2D) nickel cyanide coordination polymer precursors. The Ni3C based nanosheets have lateral length of about 200 nm and thickness of 10 nm. When doped with Fe, the Ni3C based nanosheets exhibited outstanding electrocatalytic properties for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). For example, 2 at % Fe (atomic percent) doped Ni3C nanosheets depict a low overpotential (292 mV) and a small Tafel slope (41.3 mV dec−1) for HER in KOH solution. An outstanding OER catalytic property is also achieved with a low overpotential of 275 mV and a small Tafel slope of 62 mV dec−1 in KOH solution. Such nanodot‐incorporated 2D hybrid structures can serve as an efficient bifunctional electrocatalyst for overall water splitting. |