Mesoporous Al/MCM-41 was synthesized by extracting silicon carbide sludge and granite sludge as the sources of silicon and aluminum. Different concentrations of aminosilane (2.5, 5, 7.5 vol.%) were used to reflux the grafted NH2-Al/MCM-41 with amine functional groups (NH2-Al/MCM-41). The physical and chemical characteristics were analyzed. The results confirmed that silicon carbide sludge and granite sludge can effectively synthesize Al/MCM-41 with low cost and environmental protection. Reflow grafted amine functional groups can effectively improve the surface properties of NH2-Al/MCM-41. The moisture adsorption and desorption capacity of grafted NH2-Al/MCM-41 with amine functional groups was also studied. Based on moisture adsorption and desorption capacity, the surface properties of NH2-Al/MCM-41 were studied. When 5 vol.% of NH2-Al/MCM-41 amine functional groups is added, the moisture adsorption and desorption capacity is best. When the relative humidity = 95%, the equilibrium moisture content is 39.4 kg/kg, which complies with the standard of Japanese Industrial Standard (JIS A 1475). Therefore, the use of waste derived from the industry to replace expensive commercial materials was simple and environmentally friendly, and the grafted NH2-Al/MCM-41 with amine functional groups can be utilized in multiple applications, particularly as moisture regulation materials in building engineering.