Vertically oriented graphene (VG) nanosheets exhibit unique structural characteristics, such as large accessible surface area, rich edges, high electrical conductivity, open network channels, and agglomeration resistance, for electrochemical energy‐storage applications (e. g., supercapacitors, lithium‐ion batteries, etc.). In this Review article, we summarize recent progress in the design and engineering of VG‐based electrodes for high‐performance electrochemical energy technologies within the context of energy‐storage mechanisms and charge‐transfer kinetics, and include a perspective to highlight the challenges and promises in the exploitation of vertically oriented two‐dimensional carbon nanostructures for further enhancement of the performance of electrochemical energy‐storage devices.