Methods and compositions utilizing aluminum, magnesium, and calcium-based additives for the treatment and neutralization of wastewater are described for removing contaminants from wastewater, including reducing phosphorous-containing compounds, total suspended solids (TSS), biological oxygen demand (BOD), fats, oils, and greases (FOG), and total Kjedahl nitrogen (TKN) are described. Methods and compositions to control pH, sulfur and sodium loads present in wastewater and precipitatable solids are described. Concentrations of aluminum, magnesium, and calcium-based additives are maintained at mass action concentrations to the wastewater component levels present in the wastewater and bracketed approximately +/−0.5 pH units about the pK value of the soluble, buffering species.