Low-temperature catalytic pretreatment is a promising approach to the development of an improved liquefaction process- This work is a fundamental study on effects of pretreatments on coal structure and reactivity in liquefaction. The main objectives of this project are to study the coal structural changes induced by low-temperature catalytic and thermal pretreatments by using spectroscopic techniques; and to clarify the pretreatment-induced changes in reactivity or convertibility of coals in the subsequent liquefaction. This report describes the recent progress of our work. Substantial progress has been made in the spectroscopic characterization of structure and pretreatment-liquefaction reactions of a Montana subbituminous Coal (DECS-9), and thermochemical analysis of three mw and reacted bituminous coals. Temperature programmed liquefaction has been performed on three low-rank coals both in the presence and absence of dispersed molybdenum sulfide catalyst. We also performed a detailed study of the effects of mild thermal pretreatment -- drying in air and in vacuum -- on thermal and catalytic liquefaction of a Wyodak subbituminous coal. Important information on structure and structure transformation during thermal pretreatment and liquefaction reactions of low-rank coals has been derived by applying solid-state CPMAS 13C NMR and flash pyrolysis-GC-MS (Py-GC-MS) for characterization of the macromolecular network of a Montana subbituminous coal and its residues from temperature-programmed and nonprogrammed liquefaction (TPL and N-PL) at final temperatures ranging from 300 to 425°C in H-donor and non-donor solvents. The results revealed that this coal contains significant quantities of oxygen-bearing structures, corresponding to about 18 O-bound C per 100 C atoms and one O-bound C per every 5 to 6 aromatic C.