To control and optimize the process for making ceramsite from wastewater treatment sludge (WWTS) and drinking-water treatment one (DWTS), the effect of mass ratios of (Fe 2 O 3 +CaO+MgO)/(SiO 2 +Al 2 O 3 ) (defined as F/SA ratios); SiO 2 :Al 2 O 3 and Fe 2 O 3 :CaO:MgO (under the condition of fixed F/SA ratio) on the characteristics of ceramsite were investigated. It was found that the optimal F/SA ratios for making ceramsite range 0.175–0.45. Na–Ca feldspars and amorphous phases increase in ceramsite as F/SA ratios increase. Ceramsite with porous surfaces, expanded structures, and complex crystalline phases can be obtained at 0.275≤F/SA≤0.45, which accordingly cause the decrease in compressive strength. Higher strength of ceramsite with lower porosity can be obtained at 0.175≤F/SA<0.275, and under the condition of F/SA ratio=0.275, the raw materials can produce ceramsite with desired physical properties at 18.2:35≤SiO 2 :Al 2 O 3 ≤45:10.2 and 10:2.7:1.4≤Fe 2 O 3 :CaO:MgO≤5.3:6:1.6. Ceramsite with higher compressive strength and lower porosity can be obtained at SiO 2 :Al 2 O 3 >27.2:15.8 and Fe 2 O 3 :CaO:MgO>6:3.5:1.8. Results indicate that F/SA ratios could be used as an important parameter to control the production process of ceramsite with desired physicochemical properties and resolve the disposal problems of residual sludges.