The spin-Hamiltonian parameters (g factors g//, g⊥ and hyperfine structure constants 47 Ai, 49 Ai, where i = // or ⊥, 47 Ai and 49 Ai denote the values of isotopes 47 Ti 3+ and 49 Ti 3+ ) of the Ti 3+ ions at the tetrahedral Si 4+ sites in ZrSiO4 crystal are computed from the high-order perturbation formulas based on the cluster approach where the contributions due to both the d orbitals of central d n ion and p orbitals of ligand ion are considered. The calculated results are reasonably coincident with the experimental values. The defect structure of (TiO4) 5− impurity cluster which differs from the replaced host (SiO4) 4− cluster in ZrSiO4 is evaluated in the calculation. The results are discussed.