To improve the utilization efficiency of aeolian sand, this study investigates the influence of varying calcium carbonate whisker volume fractions on the compressive and splitting tensile strengths of aeolian sand concrete. Scanning electron microscopy (SEM) and nuclear magnetic resonance (NMR) were employed to examine the interfacial bonding between whiskers and cement paste and to elucidate the strengthening mechanism. Based on the experimental results, a theoretical model of relationships among compressive strength, splitting tensile strength and curing age was established. The findings show that the incorporation of an appropriate amount of calcium carbonate whiskers significantly improves pore structure and mechanical performance. When the aeolian sand content is 60%, the optimal whisker volume fractions for compressive strength and splitting tensile strength are 0.15% and 0.20%, respectively. The proposed predictive model aligns well with the experimental data and effectively predicts strength development with age.