The use of aluminum-based coagulants in water pretreatment is being carefully considered because aluminum exposure is a risk factor for the onset of Alzheimer’s disease. Lightly burned-dolomite kiln dust (LB-DKD) was evaluated as an alternative coagulant because it contains high levels of the healthful minerals calcium and magnesium. An organic pore forming agent (OPFA) was incorporated to prepare porous granules after OPFA removal through a thermal decomposition process. A spray drying method was used to produce uniform and reproducible spherical granules with low density, since fine dolomite particles have irregular agglomeration behavior in the hydration reaction. The use of fine dolomite powder and different porosity granules led to a visible color change in raw algae (RA) containing water, from dark green to transparent colorlessness. Also, dolomite powders and granules exhibited a mean removal efficiency of 48.3% in total nitrogen (T-N), a gradual increase in the removal efficiency of total phosphorus (T-P) as granule porosity increased. We demonstrate that porous dolomite granules can improve the settling time and water quality in summer seasons for the emergent treatment of excessive algal blooms in eutrophic water.