In the present series of papers, the coherent states of Sp(2d,R), corresponding to the positive discrete series irreducible representations 〈λd+n/2,...,λ1+n/2〉 encountered in physical applications, are analyzed in detail with special emphasis on those of Sp(4,R) and Sp(6,R). The present paper discusses the unitary-operator coherent states, as defined by Klauder, Perelomov, and Gilmore. These states are parametrized by the points of the coset space Sp(2d,R)/H, where H is the stability group of the Sp(2d,R) irreducible representation lowest weight state, chosen as the reference state, and depends upon the relative values of λ1,...,λd, subject to the conditions λ1≥λ2≥ ⋅ ⋅ ⋅ ≥λd≥0. A parametrization of Sp(2d,R)/H corresponding to a factorization of the latter into a product of coset spaces Sp(2d,R)/U(d) and U(d)/H is chosen. The overlap of two coherent states is calculated, the action of the Sp(2d,R) generators on the coherent states is determined, and the explicit form of the unity resolution relation satisfied by the coherent states in the representation space of the irreducible representation is obtained. The Hilbert space of analytic functions arising from the coherent state representation is studied in detail. Finally, some applications of the formalism developed in the present paper are outlined. In particular, its relevance to the study of boson realizations of the Sp(2d,R) algebra is stressed.