Laser-ablated Th atoms react with molecular hydrogen to give thorium hydrides and their dihydrogen complexes during condensation in excess neon and hydrogen for characterization by matrix infrared spectroscopy. The ThH 2, ThH4, and ThH4(H2)x (x = 1-4) product molecules have been identified through isotopic substitution (HD, D2) and comparison to frequencies calculated by density functional theory and the coupled-cluster, singles, doubles (CCSD) method and those observed previously in solid argon. Theoretical calculations show that the Th-H bond in ThH4 is the most polarized of group 4 and uranium metal tetrahydrides, and as a result, a strong attractive "dihydrogen" interaction was found between the oppositely charged hydride and H2 ligands ThH4(H2)x. This bridge-bonded dihydrogen complex structure is different from that recently computed for tungsten and uranium hydride super dihydrogen complexes but is similar to that recently called the "dihydrogen bond" (Crabtree, R. H. Science 1998, 282, 2000). Natural electron configurations show small charge flow from the Th center to the dihydrogen ligands.