High-quality ab initio potential energy surfaces were calculated and subsequently used to predict the positions of the lowest bend-stretch vibrational states of the NO(X(2)Pi ,v=0)-Ne complex. The vibrational wavefunctions and basis set expansion coefficients, determined within the adiabatic bender model, were then used to simulate the observed spectrum for excitation of the NO(X(2)Pi ,v=2)-Ne complex. The overall position and rotational substructure matches well the experimental results for this system, which are presented in the preceding article [Y. Kim, J. Fleniken and H. Meyer, J. Chem. Phys. 114, 5577 (2001)]. A heuristic Hamiltonian, which includes the most important couplings and splittings, is used to improve the fit to experiment. (C) 2001 American Institute of Physics.