In this work, several new Mo-containing organometallic compounds (OM1, OM2, OM3, and OM4) are used as catalyst precursors in the liquefaction and hydropyrolysis of four coals of different rank (Mequinenza lignite and Wyodak, Maria Luisa, and Upper Freeport coals). Their activities are compared to those of the typically used ammonium tetrathiomolybdate (TTM). Two types of liquefaction experiments (single stage at 350 and 450 degrees C, two stage at 225-425 degrees C) were carried out, with conversions and liquid compositions being studied. For the hydropyrolysis experiments a fixed-bed reactor was used, heating at 300 degrees C up to a final temperature of 600 degrees C. Good conversions both in liquefaction and in hydropyrolysis, similar to or better than those obtained with TTM, were achieved with the pew precursors. High-rank coals are more affected by the catalytic activity promoted by the precursors.