This project addressed two main goals and one much smaller one. The main goals were (1) to improve the significance, reliability and information content in high-resolution NMR (nuclear magnetic resonance) characterization of coal samples and (2) to develop chemically informative NMR imaging techniques for coal. The minor goal was to explore advanced features of dynamic nuclear polarization (DNP) as a technique for coal characterization; this included the development of two DNP probes and the examination of DNP characteristics of various carbonaceous samples, including coals. {sup 13}C NMR advances for coal depended on large-sample MAS devices, employing either cross-polarization (CP) or direct polarization (DP) approaches. CP and DP spin dynamics and their relationships to quantitation and spin counting were elucidated. {sup 1}H NMR studies, based on CRAMPS, dipolar dephasing and saturation with perdeuteropyridine, led to a {sup 1}H NMR-based elucidation of chemical functionality in coal. {sup 1}H and {sup 13}C NMR imaging techniques, based on magic-angle spinning and rotating magnetic field gradients, were developed for introducing chemical shift information (hence, chemical detail) into the spatial imaging of coal. The TREV multiple-pulse sequence was found to be useful in the {sup 1}H CRAMPS imaging of samples like coal.