In this paper the spin-Hamiltonian parameters, g factors g//, g⊥ and zero-field splittings b20, b40, b44, b60, b64, for Gd3+ ion in molybdates AMoO4 (A=Ca, Sr, Ba, Pb) are calculated by a diagonalization (of energy matrix) method based on one-electron crystal field mechanism. The crystal field parameters in the matrix are calculated from the superposition model. The results indicate that seven calculated spin-Hamiltonian parameters are in good agreement with the experimental values by using only three reasonable adjustable parameters (i.e., the intrinsic parameters Ak (R0), where k=2, 4, 6, in the superposition model). It is shown that the diagonalization method can be used to calculate and explain the spin-Hamiltonian parameters of Gd3+ ion in crystals. The results are discussed.