Laser-ablated thorium atoms have been reacted with CO molecules during condensation in excess neon. Absorptions at 617.7 and 812.2 cm(-1) are assigned to Th-C and Th-O stretching vibrations of the CThO molecule. Absorptions at 2048.6, 1353.6, and 822.5 cm(-1) are assigned to the OThCCO molecule, which is formed by CO addition to CThO and photochemical rearrangement of Th(CO)(2). The OThCCO molecule undergoes further photoinduced rearrangement to OTh(eta(3)-CCO), which is characterized by C-C, C-O, and Th-O stretching vibrations at 1810.8, 1139.2, and 831.6 cm(-1). The Th(CO)(n) (n = 1-6) complexes are formed on deposition or on annealing. Evidence is also presented for the CThO(-) and Th(CO)(2)(-) anions, which are formed by electron capture of neutral molecules. Relativistic density functional theory (DFT) calculations of the geometry structures, vibrational frequencies, and infrared intensities strongly support the experimental assignments. It is found that CThO is an unprecedented actinide-containing carbene molecule with a triplet ground state and an unusual bent structure ( angleCThO = 109 degrees ). The OThCCO molecule has a bent structure while its rearranged product OTh(eta(3)-CCO) is found to have a unique exocyclic structure with side-bonded CCO group. We also find that both Th(CO)(2) and Th(CO)(2)(-) are, surprisingly, highly bent, with the angleC-Th-C bond angle being close to 50 degrees; the unusual geometries are the result of extremely strong Th-to-CO back-bonding, which causes significant three-centered bonding among the Th atom and the two C atoms.