We present the experimental and simulated (2+1) REMPI spectrum of the C(2)Π state of the NO-Ar complex, in the vicinity of the 3p Rydberg state of NO. Two Rydberg states of NO are expected in this energy region: the C(2)Π (3pπ) and D(2)Σ(+) (3pσ) states, and we concentrate on the former here. When the C(2)Π (3pπ) state interacts with Ar at nonlinear orientations, the symmetry is lowered to C(s), splitting the degeneracy of the (2)Π state to yield C((2)A") and C((2)A') states. For these two states of NO-Ar, we calculate potential energy surfaces using second order Møller-Plesset perturbation theory, exploiting a procedure to converge the reference Hartree-Fock wavefunction to describe the excited states, the maximum overlap method. The bound rovibrational states obtained from the surfaces are used to simulate the electronic spectrum, which is in excellent agreement with experiment, providing assignments for the observed spectral lines from the calculated rovibrational wavefunctions.