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Pillararene/calixarene-based functional materials have garnered significant attention for their unique topological/chemical structures and physicochemical properties, and their extended applications in electrochemistry have given rise to a promising area of research. This review details current advance in developing electrochemical energy materials based on pillararene/calixarene systems from the viewpoint of both fundamental theoretical simulations and research on practical applications. First, we discuss the underlying mechanisms of applying pillararene/calixarene-based systems for electrochemical energy applications. Second, we summarize simulation studies on pillarquinone and calixquinone with intrinsic structures for applications in batteries. In addition, state-of-the-art applications of pillararene/calixarene-based systems in electrochemical energy storage devices such as lithium/sodium-ion batteries and supercapacitors are highlighted. The diverse roles they play and the various design strategies that have been investigated for high-performance pillararene/calixarene-based batteries are analyzed. Finally, we discuss the prospects for further developments in this emerging field. This review not only describes recent advances in pillararene/calixarene-based batteries and supercapacitors but also lays a firm groundwork for their further application in electrochemical energy engineering.