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In this work, we report the results of a combined ab initio and experimental investigation of highly excited Σg+1 and Πg1 states of the cesium dimer in a previously unobserved energy region of the molecule. The structure of these high-lying electronic states was predicted via calculations in the framework of the pseudopotential method and observed via the optical–optical double resonance technique. Understanding the rovibronic structure of the cesium dimer at this high energy regime has significance for the formation of ultracold Cs2 ground state molecules and their detection using resonantly enhanced multiphoton ionization (REMPI) techniques. Using the ab initio results and the selection rules for dipole allowed transitions, the experimentally observed rovibrational levels were identified as belonging to the 11Σg+1 and 61Πg electronic states. The Dunham–RKR method was utilized to generate experimental potential energy curves for the two electronic states.