The modeling of the concrete matrix serves as a foundation for mesoscale analysis of concrete, which provides a crucial avenue for investigating the crack propagation and strength characteristics of concrete. However, the primary prerequisite for conducting such analyses is the generation of aggregate models. By combining the advantages of Voronoi diagrams and the random walk algorithm (RWA), a Voronoi-random walk algorithm is proposed in this paper. The algorithm overcomes the limitations of traditional methods, including constraints on aggregate volume fraction, low computational efficiency, and insufficient randomness in aggregate distribution. The meso-structure of a concrete block was modeled by the proposed method, and then its failure behavior under uniaxial compression was simulated using the finite element method. The numerical results agreed well with the experimental observations, indicating the effectiveness and accuracy of the proposed approach.