Herein, we synthesized fly ash aggregates (FAAs) through a hydrothermal synthesis process utilizing fly ash, quicklime, and cement under saturated steam conditions at 180 °C. We systematically investigated the influence and mechanisms governing the physical and mechanical properties of autoclaved FAAs by incrementally replacing cement with quicklime in 5% equal mass intervals. Our results revealed that the substitution of cement with quicklime yielded lightweight aggregates (LWAs) exhibiting water absorption ranging from 1.33% to 22.88% after 1 h and 1.67% to 26.22% after 24 h, loose bulk densities between 847 kg/m