In order to apply precipitated calcium carbonate (PCC) in the detergent industry, its ability to deposit calcium ions in hard water is an important process. In this work, the calcium ion deposition in the presence of PCC from different sources is investigated to reveal the influencing factors and mechanism of nucleation and crystal growth of CaCO3. SEM, XRD, Malvern particle size analysis, and calcium electrodes are used to evaluate the effects of PCC morphology, saturation of Ca2+, and PCC additive amount on the deposition behavior of CaCO3. Through SEM and Malvern particle size analysis, it is found that the precipitation of calcium ions is obviously accelerated by PCC acting as seeds. Moreover, calcium ions are effectively adsorbed on (211) crystal facets, thus prismatic and scalenohedral PCC crystals exhibit better adsorption performance than irregular cubic PCC ones. In addition, XRD demonstrates that PCC reduces or even eliminates the formation of crystals such as vaterite, displaying high deposition capacity under complex water conditions (slightly acidic or highly alkaline pH, low magnesium ion concentration (<0.01 M), and temperatures of 0–60 °C), forming thermodynamically stable calcite in water, which significantly controls the instability of the washing process.