Calcium phosphates were produced by mechanosynthesis, using eggshell, H3PO4 and 6–83 wt%-H2O. Mixtures were milled at 600 rpm during 0.5–12 h. Resulting calcium phosphates occur within specific milling domains; H2O concentration determines onset and stability of monophasic hydroxyapatite. Within the tested conditions, brushite is the first detected calcium phosphate precipitated from solution. In 6, 40 and 56 wt%-H2O, monetite intermediates brushite's transformation to hydroxyapatite; in 71 and 83 wt%-H2O transformation is direct. Hydroxyapatite formation is favoured at the H2O extremes tested, 6 and 83 wt%. CO2 build-up in the confined jar and nucleation-and-growth events during drying are possible obstacles upon control of morphology and composition of synthesised particles. The potential of chicken eggshell as direct biogenic source and the ability of high-energy milling as corresponding processing route to produce calcium phosphates was demonstrated. This signals a route for reliable production of brushite, monetite and hydroxyapatite. A preliminary milling map was built, allowing to obtain desired final product under specific milling conditions.