The modular multilevel converter (MMC) is the state-of-the-art for multilevel converter topologies. This study presents the operation of the MMC using the multilevel selective harmonic elimination pulse-width modulation (MSHE-PWM) technique. MSHE-PWM offers tight control of the low-order harmonics and the lowest switching frequency for the power semiconductors among all modulation techniques. A comprehensive analysis of the modulation methods for the MMC leads to two different modulation patterns for MSHE-PWM. A method for selecting the number of sub-modules in the phase-legs of the converter is also proposed in this study. Simulation results for both patterns are provided and verified through matching experimental results from a single phase 11-level laboratory prototype.