This study presents a novel technique for the controllable preparation of aragonite CaCO3 whiskers using a microdispersion process. Calcium dodecyl benzenesulfonate [Ca(Ar鈥揝O3)2] was first used as an additive for controlling the crystalline form. A homogeneous concentration distribution in the system was achieved due to the efficient micromixing. The effects of various operation parameters on the whiskers were determined, and the reaction conditions were optimized. The mechanism of the additive was discussed. The dynamic adsorption of Ca(Ar鈥揝O3)2 on the surface of whiskers was experimentally demonstrated to be in charge of maintaining the one-dimensional growth and the high purity of the crystals. Aragonite CaCO3 with a crystalline purity of 98鈥?9.5% was controllably synthesized at room temperature. The whiskers were approximately 27 渭m in length and had an aspect ratio of about 58.