The main two factors of the mechanical properties and structure of geopolymers including reactive silicon-aluminum ratios and particle fineness were investigated. Vanadium-bearing shale residue (VSR), fly ash (FA), and silica fume (SF) were subjected to alkali thermal activation (ATA) to increase the content of reactive silicon and aluminum, then a leaching experiment was carried out to quantify the content of active silica and aluminum in the raw materials, which indicated that the reactive silicon-aluminum ratios are well linearly related wit...