Chemical looping combustion (CLC) with syngas, a synthesized gas mixture of CO, H 2 , CO 2 , H 2 O(g), N 2 , and H 2 S, was investigated using thermodynamic simulation, with focus on carbon deposition and sulfur evolution in CLC. Five metal oxides, such as NiO, CuO, Fe 2 O 3 , Mn 3 O 4 , and CoO, were selected as oxygen carriers for CLC application. Different influencing factors on the formation of carbon deposits were investigated, including pressure, fuel reactor (FR) temperature, oxygen excess number Φ (denoting the availability of lattice oxygen in the oxygen carrier to the fuel), and fuel gas composition. Higher temperature and larger oxygen excess number Φ inhibited the formation of carbon deposits while the pressurized condition caused the opposite. The increase of H 2 O(g) and CO 2 fraction in syngas reduced carbon deposition while, in contrast, a larger H 2 S occurrence in syngas led to more carbon deposits to be formed. A sensitivity analysis to the different factors revealed that carbon deposition was mainly determined by the FR temperature and the oxygen carriers provided while other factors played a minor role. In addition, the predominant C-bearing species and their distributions at different temperatures were thermodynamically investigated. At low FR temperature and oxygen-deficient condition (i.e., oxygen excess number Φ < 1), the predominant carbon species as solid deposits were mainly elemental carbon or carbonates for NiO, CuO, Fe 2 O 3 , and CoO while MnC 2 and MnCO 3 were the main species for Mn 3 O 4 . In terms of the evolution of sulfur in CLC with syngas containing a basic composition of CO, N 2 , H 2 , and H 2 S, the low pressure, high temperature, and adequate lattice oxygen would make more sulfur species form in the gas phase. After that, CO 2 and H 2 O(g) were introduced into the syngas, and they were found to possibly serve as additional oxidizers to convert H 2 S into SO 2 . The oxidation function of CO 2 was slightly stronger than that of steam. Again, the evolution and distribution of various sulfur species was studied. For four metal oxides (NiO, Fe 2 O 3 , Mn 3 O 4 , and CoO), the most possible solid sulfur compounds were Ni 3 S 2 , Fe 0.84 S, MnSO 4 , and Co 0.89 S, respectively. But for CuO, at Φ < 1, Cu 2 S was the main solid sulfur compound while at Φ > 1 CuSO 4 and Cu 2 SO 4 dominated.