The process of superhard particle breakage in the grinding zone of the fluidized bed opposed jet mill is investigated using the CFD-DEM (computational fluid dynamics-discrete element method) coupling method with the Tavares UFRJ Breakage Model in the present study. The effects of structural and operational parameters, such as target plate structure, nozzle position, air inlet velocity, and feed rate, on the equipment stress distribution, airflow velocity, pressure field, particle velocity, and cumulative particle size distribution are thoroughly studied to determine the optimal structural and operational parameters. Experimental validation is conducted, including scanning electron microscope (SEM) observation of particle morphology and analysis of particle size distribution of ground product particles. The simulation results indicate that the wear rate of the structure without a target plate is lower than that of the structure with a target plate in the grinding central zone. Therefore, the structure without a target plate is chosen for further investigation. The cumulative particle size distribution after grinding is influenced by nozzle position, air inlet velocity, and feed rate. The particle D50 is positively correlated with nozzle spacing and feed rate, while it is negatively correlated with air inlet velocity. The optimal grinding effect is achieved when the distance between the nozzle and the center of the grinding zone ranges from 52.5 mm to 72.55 mm, the air inlet velocity is 950 m/s, and the feed rate is 10.5 g/s. Through experimental investigation, it has been observed that when the feed rate is 10 g/s, the particle size distribution becomes more uniform. Furthermore, consistent trends in the cumulative particle size distribution in the experiment and simulation results can be found, which validates the present numerical model. It was observed that particles at low feed rates retain certain angular edges, while particle roundness increases at high feed rates.