This paper investigates the effect of varying solid alkali activators on the fresh and hardened properties and microstructural changes of one-part geopolymers (OPGs). Single and binary solid alkali activators were used to activate high calcium fly ash. The alkali activators were either solely sodium metasilicate (Na₂SiO₃) or a combination of sodium aluminate (NaAlO₂) and sodium metasilicate (Na₂SiO₃). The OPG activated with anhydrous Na₂SiO₃ achieved an excellent 28-day compressive strength of 83.6 MPa while OPG activated with NaAlO₂ and Na₂SiO₃ attained a compressive strength of 45.1 MPa. The Na₂SiO₃-activated OPG demonstrated better fluidity than the OPG activated with NaAlO₂ and Na₂SiO₃ due to the thixotropic behaviour caused by the NaAlO₂. The Na₂SiO₃-activated OPG consisted of sodium-calcium aluminium silicate hydrate ((N,C)-A-S-H) gel phase, while the OPG activated with NaAlO₂ and Na₂SiO₃ comprised of the coexistence of sodium aluminium silicate hydrate (N-A-S-H) and calcium aluminium silicate hydrate (C-A-S-H) gel phases. Regardless of the distinctive properties, the OPGs are adequate for building materials applications.