The phase-shifted-carrier (PSC) technique is preferred for multilevel converters in medium-voltage applications with low submodule (SM) number. This technique can elevate the equivalent switching frequency resulting in low total harmonic distortions. However, for half-/full-bridge hybrid modular multilevel converter (MMC) with boosted modulation index, the conventional PSC method is invalid due to the asymmetric voltage reference wave. The SM capacitor voltages deviate from the rated value and harmonics below equivalent switching frequency appear in the arm and equivalent ac voltages. This paper introduces an improved PSC technique with a capacitor sorting algorithm to overcome this problem. The negative part of the reference wave is turned over and then multiplied by a correction factor. The angular displacement for triangular carriers between the upper and lower arms is determined by the parity of the half-bridge number per arm. With the proposed method, the capacitor voltages are balanced and the ac voltage of MMC has the lowest harmonic distortion. Double-Fourier analysis for the proposed technique is carried out, and harmonic characteristics are revealed. The experimental results validate the correctness and feasibility of the improved PSC technique for hybrid MMC with boosted modulation index and asymmetric reference wave.