We present new results from experimental studies of high-lying electronic states of the NaCs molecule that are currently underway in our laboratory. The optical-optical double resonance method is used to obtain Doppler-free excitation spectra for several excited states. Selected data from the 53Π0, 43Π0 and other high lying electronic states are used to obtain Rydberg-Klein-Rees (RKR) and Inverse Perturbation Approach (IPA) potential curves. Small oscillations in the other wall of the 53Π0 potential suggest strong interactions with other electronic states. A modified version of Le Roy’s BCONT program was used to simulate NaCs 53Π0 → 1(a) 3Σ + bound-free emission spectra. These simulations were used to fit the experimental spectra with a parameterized 1(a) 3Σ + repulsive wall and the 53Π0 → 1(a) 3Σ + transition dipole moment function, µ(R). The fitted µ(R) is in good agreement with the theoretical transition dipole moment function of Aymar and Dulieu [Mol.Phys. 105, 1733 (2007)]. In related work, we have identified additional electronic states which we have tentatively assigned as the 43Π0 and 53Π1 (and possibly the 53Π2) electronic states of NaCs.