Vapor phase carbonylation of ethanol with Ni/C and Ni-Zn/C catalyst was investigated under atmospheric pressure. Ni-Zn/C was found to have a significantly higher activity and selectivity than Ni/C. Effects of Zn and Ni loading on ethanol conversion and product distributions were also investigated, and the sequence of metal loading was compared. The catalyst was characterized by XRD (X-ray diffraction) and SEM-EDS. The spectra of XRD demonstrated that the catalyst structure was changed from crystalline to non-crystalline in the process of carbonylation. Stable iodide compound was formed due to the interaction between C2H5I and active metals. The authors believe that the active phase of carbonylation might have been non-crystalline.