Nanostructured carbon materials, especially activated carbon, carbon nanotubes, and graphene, have been widely studied for supercapacitor applications. To maximize the efficacy of these materials for electrochemical energy storage, a detailed understanding of the relationship between the nanostructure of these materials and their performance as supercapacitors is required. A fundamental structural parameter obtained from the Raman spectra of these materials, the in-plane correlation length or nanocrystalline domain size, is found to correlate with the electrochemical capacitance, regardless of other morphological features. This correlation for a common nanostructural characteristic is believed to be the first result of its kind to span several distinct nanostructured carbon morphologies, including graphene-carbon nanotubes hybrid materials, and may allow more effective nanoscale engineering of supercapacitor electrode materials.