The present study investigated geopolymerization in alkali-activated fly ash under elevated pressure conditions. The fly ash was activated using either sodium hydroxide or a combination of sodium silicate solution and sodium hydroxide, and was cured at 120 degrees C at a pressure of 0.22 MPa for the first 24 h. The pressure-induced evolution of the binder gel in the alkali-activated fly ash was investigated by employing synchrotron X-ray diffraction and solid-state Si-29 and Al-27 MAS NMR spectroscopy. The results showed that the reactivity of the raw fly ash and the growth of the zeolite crystals were significantly enhanced in the samples activated with sodium hydroxide. In contrast, the effects of the elevated pressure conditions were found to be less apparent in the samples activated with the sodium silicate solution. These results may have important implications for the binder design of geopolymers, since the crystallization of geopolymers relates highly to its long-term properties and functionality.