Alkali-activated materials (AAMs) are currently being pursued as viable alternatives to conventional ordinary Portland cement because of their lower carbon footprint and established mechanical performance. However, our understanding of the mesoscale morphology (∼1 to 100 nm) of AAMs and related amorphous aluminosilicate gels, including the development of the three-dimensional aluminosilicate network and nanoscale porosity, is severely limited. This study investigates the structural changes that occur during the formation of AAM gels at the mesoscale by utilizing a coarse-grained Monte Carlo (CGMC) modeling technique that exploits density functional theory calculations. The model is capable of simulating the reaction of an aluminosilicate particle in a highly alkaline solution (sodium hydroxide or sodium silicate). Two precursor morphologies have been investigated (layered alumina and silica sheets mimicking metakaolin and spherical aluminosilicate particles reminiscent of coal-derived fly ash) to determine if the precursor morphology has an impact on the structural evolution of the resulting alkali-activated aluminosilicate gel. The CGMC model can capture the three major stages of the alkali-activation process-dissolution, polycondensation, and reorganization-revealing that the dissolved silicate and aluminate species, ranging from monomers to nanoprecipitates (100s of monomers in size), exist in the pore solution of the hardened gel. The model also reveals that the silica concentration of the activating solution controls the extent of dissolution of the precursor particle. From the analysis of the aluminosilicate cluster size distributions, the mechanisms of AAM gel growth have been elucidated, revealing that Ostwald ripening occurs in systems containing free silica at the start of the reaction. On the other hand, growth of the hydroxide-activated systems (metakaolin and fly ash) occurs via the formation of intermediate-sized clusters in addition to continual growth of the largest particle. The simulation results indicate that the nature of the gel growth is not influenced by the precursor particle morphology.