In this study, the planetary ball milling with CaO addition was used to remediate lindane-contaminated soil. Based on Hertzian theory, a mathematical model was proposed to simulate the trajectory of grinding ball and the local energy transfer during a planetary operation at the disk rotation velocities of 150–250 rpm. Besides, the influence of different parameters on lindane removal in soil was investigated, whose results showed that disk rotation velocity and reagent-to-soil ratio had a positive effect, while soil moisture, initial concentration of lindane, and mass of polluted soil demonstrated a negative influence. The mechanochemical method exhibited a higher degradation performance at 3 wt% CaO addition, and a disk rotation velocity of 250 rpm. Active species generated by ball collisions in the presence of CaO, especially superoxide (·O2−) demonstrated a significant role in participating in the lindane conversion. In combination with GCMS and XPS analysis, the proposed model provides insight into mechanochemical remediation process from physical and chemical perspectives, which mainly includes four main steps: mixing, inducing, chemical reaction, and structure destruction.