As an excellent class of electrode materials, carbon‐based materials have garnered sustained attention. Constructing carbon‐based skeleton with unique structure has become a vital research area in the fields of electrocatalysis. Recently, surface curvature has been extensive discussed as a compelling factor in electronic modulation for electrocatalyst design. Benefitting from its distinctive regulation, the intrinsic activity and service stability of catalysts during electrocatalytic process can be significantly improved. Therefore, a helical structure that adeptly integrates well‐regulated, highly ordered surface curvatures is considered to be of great research value for the synthesis of carbon‐based skeleton. In this Concept article, we systematically summarize the up‐to‐date reports on the synthetic methods of carbon‐based skeletons with helical structures and present major challenges in this field. We also emphasize that the helical carbon‐based skeleton could be combined with transition metals for cooperative coupling, potentially leading to the further development of high‐efficiency electrocatalysts.