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White mud is residue discharged during the acid method in the aluminum extraction process from coal fly ash, and this material is harmful to the environment. The implementation of an environmentally friendly and valuable way to use white mud is a key factor restricting the commercial application of the acid method in the fly ash alumina extraction technology. An analysis of white mud revealed the following: (1) it was highly enriched in SiO2 (70–80%) while concentrations of acid-soluble elements, such as Na, Al, and Fe, and some hazardous heavy metals, including Pb and Cr, were significantly lower than raw fly ash; (2) approximately 80% of SiO2 had relatively high reaction activity because of the foregoing Al-extraction treatment. Through an ingenious green chemical process, the complete conversion of white mud into silicon–calcium fertilizer (SCF) was achieved under very mild reaction conditions (approximately 100 °C and atmospheric pressure). Waste liquor was totally recycled, and no secondary solid waste was generated. The SCF had an available silicon content (ASC) of 35%, significantly higher than the commercial standard (20%). Converting them into soil conditioners or ecological remediation materials with the lowest possible energy consumption and secondary pollution may be the most promising approach for the future disposal of aluminosilicate industrial solid wastes. [ABSTRACT FROM AUTHOR]