To reduce stored capacitor energy in modular multilevel converters (MMCs), previous papers propose injection of harmonics in the arm circulating currents and zero-sequence voltages. While this approach is effective, previously utilized combinations of injected harmonics significantly increase converter current ratings. In contrast, the optimization approach developed in this article identifies harmonics that simultaneously achieve capacitor energy optimization and reduced overrating of converter currents. In addition, the proposed approach eliminates the possibility of convergence to local minima, which is a significant improvement on previously proposed nonconvex optimization approaches. Experimental verification of the proposed approach is performed on a low-voltage three-phase modular multilevel converter.