The drastic variations in thermal properties of supercritical CO2 near its pseudo-critical point induce the formation of complex boundary layer structures within pipelines, rendering it susceptible to heat transfer deterioration under the influence of buoyancy forces. The Helmholtz self-excited cavity can generate self-excited pulsating jets, enhancing the intermixing between fluids inside the heat exchanger tubes, disrupting the thermal boundary layer, and suppressing heat transfer deterioration. In this study, the characteristics and mechanisms of self-excited oscillations of supercritical CO2 flowing vertically upward in the Helmholtz self-excited cavity were investigated using the large eddy simulation (LES) method. A detailed analysis of cavitation and vortex evolution within the cavity was conducted, along with an exploration of the influence of inlet pressure and structural parameters on the frequency characteristics of pulsations. The results indicate a close relationship between cavitation and vortex interactions and the pulsation frequency. An increase in inlet pressure leads to a significant cavitation phenomenon near the jet shear layer and an increase in vortex frequency. Dimensionless cavity length (Lc/d1) enlargement results in an increase in outlet pulsation frequency but a decrease in pulsation amplitude. The critical dimensionless ratio of cavity diameter (Dc/d1) plays a crucial role in maintaining the desired pulsation frequency and amplitude. Within the working range outlined in this paper, practical insights for system design and operation are provided by the optimal parameters of Lc/d1 = 3 and Dc/d1 = 10.