The triplet potential energy surface of the O(P-3) + CS2 reaction is investigated by using various quantum chemical methods including CCSD(T), QCISD(T), CCSD, QCISD, G3B3, MPWB1K, BB1K, MP2, and B3LYP. The thermal rate coefficients for the formation of three major products, CS + SO ((3)Sigma(-)), OCS + S (P-3) and CO + S-2 ((3)Sigma(-)(g)) were computed by using transition state and RRKM statistical rate theories over the temperature range of 200-2000 K. The computed k(SO + CS) by using high-level quantum chemical methods is in accordance with the available experimental data. The calculated rate coefficients for the formation of OCS + S (P-3) and CO + S-2 ((3)Sigma(-)(g)) are much lower than k(SO + CS); hence, it is predicted that these two product channels do not contribute significantly to the overall rate coefficient.