In synthetic fabrication, the process parameters decide the growth nucleation, phase translation, and the evolution of morphological facets of nanostructured materials. This work demonstrates the formation of different crystallographic phases of calcium phosphate by the influence of pH from acidic to alkaline conditions and also investigated their bone regeneration, protein adsorption, and pro‐angiogenic properties. Present results illustrate that the alteration of pH is the crucial factor for the synthesis of calcium phosphate (CP) phases. The structural analysis reveals the monetite (CaHPO4) phase with a triclinic crystal system for pH 5, dual‐phase of monetite combined with hydroxyapatite at the neutral pH 7, and pure phase of hydroxyapatite (Ca10[PO4]6OH2) with hexagonal structure at pH 10. Microscopic analysis portrays the cubic and rod‐like morphologies by changing the pH values. FTIR and RAMAN spectroscopic analyses confirm the stretching, bending, and vibrational modes of dominant phosphate groups of different CP phases. Further, the biocompatibility of the prepared CP phases was examined by hemolysis assay, which showed less than 2% of lysis and enhanced cell viability. Moreover, the bioactivity study revealed rapid mineralization and a higher protein adsorption rate for the monetite CP phase (M‐CP). Subsequently, the chick embryo angiogenesis assay elucidated 33% higher neovascularization for M‐CP compared with the other two CP phases. The fabricated M‐CP nanostructure constitutes a promising candidate for biomedical applications.