Graphene is a competitive electrode material for supercapacitors due to its unique two-dimensional structure,large surface area,high conductivity,and good physicochemical stability.However,random agglomeration and restacking of graphene sheets result in a reduced surface area and a loose structure with low density,which severely restricts the application for high gravimetric/volumetric energy density devices.Rational design of the layered-stacking structure of graphene assemblies can effectively prevent the restacking of graphene sheets,construct efficient ion transport channels,and improve spatial utiliza-tion,demonstrating the huge potential for developing advanced electrode materials.Herein,from the aspect of improving the electrochemical kinetics through designing efficient electron and ion transport paths,we first highlight the advantages of layered-stacking graphene assemblies,describe some com-mon routes for preparing graphene building units,and then summarize the novel methods to design layered-stacking structures.A comprehensive review of the typical structure including nanocarbon pil-lared graphene,porous graphene blocks,and graphene ribbon films is provided with a focus on the mechanisms behind the performance improvements.Finally,critical challenges and some general ideas for future development are proposed,which may open up new opportunities for material chemistry and device innovation.