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The voids in coarse aggregate (VCA) is an important volumetric index in the mineral aggregate gradation design of stone matrix asphalt (SMA) mixtures. To explore the law of variation for VCA formed by the packing of basalt and lime coarse aggregates, a uniform design method and vibrating compaction tests were used to establish the prediction model. Based on the test results and stepwise regression analysis, a reliable prediction model of VCA was obtained. There is a multiple nonlinear relationship between the VCA and the proportion of each coarse aggregate in the mixture. Regardless of the type of coarse aggregates used, the rule of VCA with different forms of aggregate gradation curves has universal significance. This conclusion can help to determine the aggregate gradation in the design of SMA mixtures.