Interest is growing in nanoparticles made of earth abundant materials, like alumino(silicate) minerals. Their applications are expanding to include catalysis, carbon sequestration reactions, and medical applications. It remains unclear, however, what factors control their formation and abundance during laboratory synthesis or on a larger industrial scale. This work investigates the complex system of physicochemical conditions that influence the formation of nanosized alumino(silicate) minerals. Samples were synthesized and analyzed by powder X-ray diffraction, in situ and ex situ small angle X-ray scattering, and transmission electron microscopy. Regression analyses combined with linear combination fitting of powder diffraction patterns was used to model the influence of different synthesis conditions including concentration, hydrolysis ratio and rate, and Al : Si elemental ratio on the particle size of the initial precipitate and on the phase abundances of the final products. These models show that hydrolysis ratio has the strongest control on the overall phase composition, while the starting reagent concentration also plays a vital role. For imogolite nanotubes, we determine that increasing concentration, and relatively high or low hydrolysis limit nanotube production. A strong relationship is also observed between the distribution of nanostructured phases and the size of precursor particles. The confidences were >99% for all linear regression models and explained up to 85% of the data variance in the case of imogolite. Additionally, the models consistently predict resulting data from other experimental studies. These results demonstrate the use of an approach to understand complex chemical systems with competing influences and provide insight into the formation of several nanosized alumino(silicate) phases.