This work considers the application of Wilson and NRTL equations in the multicomponent VLE prediction. We emphasize the critical comparison of partially miscible solution treatment by these two equations. Results revealed NRTL equation performed slightly better than the Wilson equation in data credibility so far as the systems examined are concerned. Estimation of optimum NRTL parameters requires further exploration. Optimization methods of pattern search, gradient search and golden section were employed in this study. All of the computations were performed on an IBM 1130 digital computer.