Because hydrological models are so important for addressing environmental problems, parameter calibration is a fundamental task for applying them. A broadly used method for obtaining model parameters for the past 20 years is the evolutionary algorithm. This approach can estimate a set of unknown model parameters by simulating the evolution process. The ant colony optimization (ACO) algorithm is a type of evolutionary algorithm that has shown a strong ability in tackling combinatorial problems and is suitable for hydrological model calibration. In this study, an ACO based on the grid partitioning strategy was applied to the parameter calibration of the variable infiltration capacity (VIC) model for the Upper Heihe River basin and Xitiaoxi River basin, China. The shuffled complex evolution (SCE-UA) algorithm was used to test the applicability of the ACO. The results show that ACO is capable of model calibration of the VIC model; the Nash–Sutcliffe coefficient of efficiency is 0.62 and 0.81 in calibration and 0.65 and 0.86 in validation for the Upper Heihe River basin and Xitiaoxi River basin respectively, which are similar to the SCE-UA results. Despite the encouraging results obtained thus far, further studies could still be performed on the parameter optimization of an ACO to enlarge its applicability to more distributed hydrological models.