As the series environmental pollution and energy crisis, and the growth of energy demand, it is very essential to develop novel energy storage device to replace traditional fossil fuels. Supercapacitors has been considered as a prospective energy storage device with broad application prospects due to the high power density, long cycle life, wide temperature range, high safety and environmental friendliness. However, the energy density of supercapacitors (E=1/2CV2) cannot meet the application requirements owing to the relatively low specific capacitance (C) and small voltage window (V). This review summarizes the strategies for designing and optimizing inorganic layered hydroxides to enhance the specific capacitance by morphology and crystal structure regulation, respectively. We also expound our viewpoints on the future development prospects of the layered hydroxides for energy storage applications.