The development of advanced electrode materials for the next generation of electrochemical energy storage (EES) solutions has attracted profound research attention as a key enabling technology toward decarbonization and electrification of transportation. Since the discovery of graphene's remarkable properties, 2D nanomaterials, derivatives, and heterostructures thereof, have emerged as some of the most promising electrode components in batteries and supercapacitors owing to their unique and tunable physical, chemical, and electronic properties, commonly not observed in their 3D counterparts. This review particularly focuses on recent advances in EES technologies related to 2D crystals originating from non‐layered 3D solids (non‐van der Waals; nvdW) and their hallmark features pertaining to this field of application. Emphasis is given to the methods and challenges in top‐down and bottom‐up strategies toward nvdW 2D sheets and their influence on the materials’ features, such as charge transport properties, functionalization, or adsorption dynamics. The exciting advances in nvdW 2D‐based electrode materials of different compositions and mechanisms of operation in EES are discussed. Finally, the opportunities and challenges of nvdW 2D systems are highlighted not only in electrochemical energy storage but also in other applications, including spintronics, magnetism, and catalysis.