In this paper, a novel non-uniformly structured surface with primary and secondary pillars is conceived to be coupled with the action of an electric field to enhance pool boiling under reduced gravity. On the surface, the secondary pillars are distributed diagonally. A three-dimensional thermal lattice Boltzmann (LB) model combined with an electric field model is employed to investigate the boiling heat transfer performance on the non-uniformly pillar-structured surface and the associated boiling enhancement mechanism. It is found that the synergistic effect of the non-uniform surface structure and the electric field leads to a non-equilibrium electric force that causes the bubbles to be pushed away from the center of the heating surface, which promotes an earlier departure of the bubbles and provides more paths for the fresh liquid replenishment. As a result, the boiling performance under reduced gravity can be significantly enhanced by utilizing such a synergistic effect, with both the critical heat flux (CHF) and the maximum heat transfer coefficient (HTC) on the non-uniformly pillar-structured surface exceeding those on a uniformly pillar-structured surface under normal gravity. Moreover, the influences of the distribution of the secondary pillars on the boiling performance under reduced gravity are also studied. It is shown that the non-uniformly pillar-structured surface whose secondary pillars are distributed diagonally performs much better than those with the secondary pillars being distributed crossly and centrally, and the synergistic effect of the non-uniform surface structure and the electric field results from tuning the distribution of the non-uniform electric force.