In the present work, a new, low energy consumption sol–gel synthesis route has been developed for geopolymer composites. Instead of the typically published 0.1–1.0 Al/Si molar ratios, the efforts of this study concentrated on the realization of >2.5 Al/Si molar ratios in the composite systems. The higher Al molar ratio significantly improves the mechanical properties. A very important aim was also the recycling of industrial waste materials with attention to environmentally friendly requirements. The very dangerous, toxic red mud as a waste product of aluminum industrial fabrication was selected for reclamation. The structural investigation was carried out by 27Al MAS NMR, XRD, and thermal analysis. The structural examination has unambiguously proven the composite phases in both gel and solid systems. The characterization of composites was performed with mechanical strength and water solubility measurements.