We have developed expertise in the detailed and quantitative NMR characterization of highly aromatic carbon materials, some with applications in catalysis. Studies of biochars, carbon-coated mesoporous oxides, and melanoidins formed in the Maillard reaction [J. Agric. Food Chem. 2009, 2011; Chem. Mater. 2014] fall into this category. Solid-state 13C NMR is the best available method for characterizing these materials comprehensively, quantifying the aromaticity and functional group concentrations, and characterizing the size of clusters of fused aromatic rings. When these materials are made from 13C-enriched precursors, distinction of heterocycles and identification of many different linkages is possible, best in spectrally edited two-dimensional 13C-13C experiments without diagonal ridge. We have developed an approach to “translate” the NMR spectra into realistic structural models of the typical repeat unit of complex organic materials. [Carbon, 2014]