Ni(3+) doped NiTi layered double hydroxide (NiTi-LDH) monolayer nanosheets with a particle size of ∼ 20 nm and a thickness of ∼ 0.9 nm have been successfully prepared through a facile bottom-up approach. These NiTi-LDH monolayer nanosheets exhibit excellent supercapacitor performance, including a high specific pseudocapacitance (2310 F g(-1) at 1.5 A g(-1)) and long durability compared with bulk LDH, owing to highly exposed conductive Ni(3+) species (NiOOH) which lead to the increased mobility rate of surface charge and electrolyte-transfer. Therefore, this work is expected to take a significant step towards exploring novel 2D monolayer electrode materials with unique physical and chemical properties for applications in energy storage and conversion.