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As a common molecule in biomineralization, L-aspartic acid (L-Asp) has been proven to be able to induce in vitro CaCO3 precipitation, but its application in sand reinforcement has never been studied. In this study, L-Asp was employed in sand reinforcement for the first time through the newly developed biomimetic carbonate precipitation (BCP) technique. Specimens with different number of BCP spray cycles were prepared, and a series of direct shear tests were conducted to investigate the impact of spray number on shear strength, critical displacement, and residual strength. Then a simplified power model for shear stress–displacement behavior was established and calibrated with the measured data. The results show that BCP can significantly improve the shear strength of sand. As the number of spray cycles increases, both the shear strength and residual strength increase, while the critical displacement decreases. Such variations can be described with two sigmoid models and a linear model, respectively. The simplified power model performs well in most cases, especially at higher spray numbers. This study is expected to provide a practical model for the shear behavior of BCP-treated mortar.