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In recent years, research on the safe utilization and green remediation of contaminated soil by intercropping has become common. In this study, the growth of an intercropping system of <i>Luffa cylindrica</i>–<i>Semen cassiae</i> in soil contaminated with medium amounts of arsenic (As) was studied using field (91.60 mg kg⁻¹) and pot (83.34 mg kg⁻¹) experiments. The field experiments showed that intercropping significantly increased the yield per plant of <i>L. cylindrica</i> by 27.36%, while the yield per plant of <i>S. cassiae</i> decreased by 21.66%; however, this difference was not significant. Intercropping reduced the concentration of As in all organs of <i>L. cylindrica</i> but increased the concentration of As in all parts of <i>S. cassiae</i>. The accumulation of As per plant of <i>L. cylindrica</i> was reduced by 20.72%, while that in a single plant of <i>S. cassiae</i> was increased by 201.93%. In addition, the concentration of As in the fruit of these two crops in these two planting modes was low enough to meet the National Food Safety Standard of China (GB2762-2017). In addition, the land equivalent ratio and As metal removal equivalent ratio of the intercropping mode was 1.03 and 2.34, indicating that the intercropping mode had advantages in land use and As removal. In the pot experiment, the biomass and As concentration of <i>L. cylindrica</i> and <i>S. cassiae</i> were roughly consistent with those in the field experiment. During the sampling period, intercropping reduced the concentration of As in the rhizosphere soil solution of <i>L. cylindrica</i> by 3.1–23.77%, while it increased the concentration of As in the rhizosphere soil solution of <i>S. cassiae</i> by 13.30–59.40%. The changes in pH and redox potential were also closely related to the content of water-soluble As in the rhizosphere environment, which affects the absorption of As by plants. In general, the <i>L. cylindrica</i>–<i>S. cassiae</i> intercropping system is a planting mode that can effectively treat soil that is moderately contaminated with As and remove it from the soil to an extent.