Micron-sized SrSO4 particles having mono-dispersed/narrow distributions have been produced with a double-jet semi-batch reactive crystallizer. Slow molar feedings over a short time maintained proper supersaturation levels and result in narrow distributions due to the prevention of agglomeration growth of small primary precipitates. Furthermore, polyethylenimine (PEI) is a suitable growth/agglomeration inhibitor for sulfate precipitation, e. g., SrSO4 and PbSO4, and effectively reduced particle sizes leading to single-micron products. Besides feeding conditions, in the present work, the influence of PEI dosage on crystal size distributions (CSDs) is investigated. The controlled double-jet feeding using a polyelectrolyte additive such as PEI will be a powerful methodology to obtain agglomeration-free uniform micro-powders as a final solid product.