Structurally stable β-Ca3(PO4)2/t-ZrO2 composite mixtures with the aid of Dy3+ stabilizer were accomplished at 1500°C. The precursors comprising Ca2+, P5+, Zr4+, and Dy3+ have been varied to obtain five different combinations. The results revealed the fact that complete phase transformation of calcium-deficient apatite to β-Ca3(PO4)2 occurred only at 1300°C, whereas the evidence of t-ZrO2 crystallization is obvious at 900°C. The dual occupancy of Dy3+ at β-Ca3(PO4)2 and t-ZrO2 structures was evident; however, Dy3+ initially prefers to occupy β-Ca3(PO4)2 lattice until its saturation limit and thereafter accommodates at the lattice site of ZrO2. The typical absorption and emission behavior of Dy3+ were noticed in all the systems and, moreover, the surrounding symmetry of Dy3+ domains has been determined from the luminescence study. All the systems ensured paramagnetic response that is generally contributed by the presence of Dy3+. A gradual increment in the phase content of t-ZrO2 in the composite mixtures ensured a significant improvement in the hardness and Young's modulus of the investigated compositions. © 2020 The American Ceramic Society