This study investigates a controlled synthesis and particle size optimization of nanocalcite particles using phosphogypsum, a waste byproduct from the phosphate fertilizer industry, and cesium carbonate (Cs₂CO₃), a common carbonate source. The effects of synthesis parameters, including temperature and pH, on the size, morphology, and crystallinity of the synthesized nanocalcite particles were systematically examined. The optimized synthesis conditions for obtaining nanocalcite particles with desired properties are discussed. The synthesized nanocalcite particles were characterized using various techniques, such as XRD, FTIR, and SEM, to analyze their crystal structure, morphology, and elemental composition. Particle sizes were determined using the Debye–Scherrer method, and accordingly, nanometric sizes were achieved. The potential applications of the synthesized nanocalcite particles in cementitious materials, agriculture, and drug delivery are highlighted. This research provides valuable insights into the sustainable synthesis and size optimization of nanocalcite particles from phosphogypsum and Cs₂CO₃ at a controlled temperature and pH.