In an earlier article [Found. Phys. 30, 1191 (2000)], a quasiclassical phase space approximation for quantum projection operators was presented, whose accuracy increases in the limit of large basis size (projection subspace dimensionality). In a second paper [J. Chem. Phys. 111, 4869 (1999)], this approximation was used to generate a nearly optimal direct-product basis for representing an arbitrary (Cartesian) quantum Hamiltonian, within a given energy range of interest. From a few reduced-dimensional integrals, the method determines the optimal 1D marginal Hamiltonians, whose eigenstates comprise the direct-product basis. In the present paper, this phase space optimized direct-product basis method is generalized to incorporate non-Cartesian coordinate spaces, composed of radii and angles, that arise in molecular applications. Analytical results are presented for certain standard systems, including rigid rotors, and three-body vibrators.