This paper investigates the processes of droplet condensation and self-propelled jumping on microcolumn-structured superhydrophobic surfaces with various size parameters. Using a three-dimensional (3D) multiphase lattice Boltzmann method, a novel phenomenon of secondary coalescence jumping is identified, and the underlying mechanisms are analyzed in detail. The simulation results show that wettability has a significant influence on droplet jumping. As the hydrophobicity of the surface increases, the droplets tend to jump from the substrate. However, structure parameters, such as the microcolumn spacing and height, have non-monotonic effects on droplet jumping. The structure parameters determine whether droplet coalescence occurs under the bottom–bottom droplet coalescence mode or the bottom–top droplet coalescence mode. Bottom–bottom droplet coalescence is shown to promote droplet jumping. Based on the simulation results and kinetic analysis, the optimal spacing-to-width and height-to-width ratios of the microcolumns for droplet jumping are found to be approximately 0.6 and 1.0, respectively. We believe the results of this work will provide valuable guidance in the design of self-cleaning surfaces and enhancing heat transfer efficiency.