This study introduces a strategy to improve the effectiveness of Cuckoo Search (CS) algorithm for the unconstrained Gibbs free energy minimization in phase equilibrium calculations of nonreactive systems. Specifically, the gradient information of the unconstrained Gibbs free energy function, which is readily available, is used to enhance the balance between diversification and intensification stages of the CS algorithm for phase-split calculations in multicomponent systems. The results showed that it is feasible to improve the numerical performance of the CS algorithm using the gradient information of the Gibbs free energy function; this improved method provides better results for phase equilibrium calculations in nonreactive systems with insignificant additional computational effort. This gradient-based Cuckoo Search (GBCS) algorithm outperformed the conventional CS algorithm, in terms of its reliability and efficiency in solving phase equilibrium problems, especially for multicomponent systems.