In this paper, the effect of harmonic voltage on partial discharge properties of LN2/PPLP (Liquid nitrogen/ Polypropylene-Laminated-Paper) insulation system for high-temperature superconducting (HTS) DC cable is studied. The harmonic components with a frequency from 50 to 350 Hz are superimposed on the DC voltage to analyze the mechanism of the harmonic amplitude and order on partial discharge (PD). The experimental results show that when the Vrms of the composite voltage remains consistent, the increase in the proportion of the harmonic amplitude will cause the enhancement of partial discharge amplitude, discharge counts and pulse repetition rate, especially as the amplitude of harmonic component exceeds that of DC voltage. The increase of the harmonic order results in variation of the derivative of the applied voltage with time (dv/dt) along the phase, which further causes the pulse repetition rate to increase. It is concluded that the harmonic components superimposed on DC voltage promote the occurrence of PD, which poses a significant threat to the insulation of superconducting DC cable.