Zeolites were synthesized from fly ash using modified one-stage method. The changes in cation exchange capacity (CEC) and chemical elements of zeolite were investigated during the synthesis process to reveal the materials and elements transformation in solid-liquid system. The approaches of XRD, SEM and FTIR were used to indicate the crystallization characteristics and mechanism. The zeolite NaP1 was synthesized, and the CEC value reached to the maximum of 135 mmol/100g at 24 h. After the hydrothermal reaction for 12 h, the characteristic peak and metastable crystalline structure of zeolite NaP1 appeared, then the hydroxy sodalite products formed at 48 h. The crystallization process was the result of materials transformation: the elements of fly ash released into the liquid system for the melting effect of alkali solution, and the solid system played the role of skeleton in crystallization process, being the “source” and the “sink” of the reaction, respectively, and the achievements presented the crystallization mechanism of liquid-phase and solid-phase transformation.