Atropine (AT) is a tropane alkaloid used as an anticholinergic drug. AT is abundantly in Datura plant seeds. In work: Zn/Mg bimetallic MOF integrated with Fe3O4, and Fe3O4@Zn/Mg MOF (Fe3O4@MOF) composite was synthesized. The compound has a high peroxidase‐like activity in the chemiluminescence (CL) reaction. The synergistic effect of Zn, Fe, and Mg metals in the Fenton reaction causes the production of reactive oxygen species (ROS), resulting in high CL intensity. Addition of AT quenching CL and thus AT can be measured. The linear range and limit of detection (LOD) for measuring AT standard solution are 5‐600μgL‐1 and 2×10‐2μgL‐1, respectively. This method is easy, fast, reversible, and selective, without biodegradability effects, low cost, high accuracy, and precision for measuring AT in the Datura plant.