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Sustainable hydraulic cements based on alkali aluminosilicate chemistry were developed with market-limited wastes acting as the primary aluminosilicate precursors. Two sets of formulations were developed with waste brick or impounded coal ash used at relatively large volume as aluminosilicate precursors. Supplementary materials were used to produce raw materials of viable chemistry. Blends of raw materials were transformed into hydraulic cements by input of mechanical energy without resorting to elevated temperatures. The resultant hydraulic cements exhibited viable strength development characteristics. FTIR, SEM, EDS and NMR analyses were conducted in order to gain insight into the structure of the hydraulic cements and their hydration products. The results pointed at the prevalence of calcium aluminosilicate hydrates among the products of hydration which thoroughly bound the non-hydrated cores of cement particles.