<p>To broaden the disposal strategy of silicate wastes, a hydrothermal method inspired by previous work on the extraction of potassium from K-feldspar was proposed in this work to handle the representative silicates of feldspars, pyrophyllite, coal gangue, coal fly ash, and as a result, two typical small zeolites of analcime and hydroxycancrinite were obtained. Systematic ion exchange experiments under the existences of Li⁺, Na⁺, K⁺, Ca²⁺, Mg²⁺ in different conditions were conducted to evaluate their cation selectivity and capability. Results showed that Li⁺ was the only cation having positive feedback on the zeolite structure, in mixed-ion system solutions, it achieved efficient lithium silicate immobilization with a Li₂O content of 4.50 <i>wt.</i>%, while in a single-ion system (LiCl solution), the Li₂O content reached 9.40 <i>wt.</i>%. The immobilization capacities in both systems surpassed those of high-grade granitic pegmatite-type lithium ores (1.5–4 <i>wt.</i>%). The structure of hydroxycancrinite is always the same before and after ion exchange, and all of them are shelf silicate structures. The Spectral analysis identified the formation of Li-zeolite from hydroxycancrinite with the successful trapping of Li⁺ inside. The overall handling process provided a new way for the process of universal silicate wastes with further combination of lithium extraction from mixed cation solution system.</p>