The challenges of handling user-hostile alkaline solutions in the conventional alkali-activated binders (AAB) have initiated the development of “just add water” or one-part solid-based AAB systems. This paper aims to present a preliminary investigation on the development of one-part ambient-cured alkali-activated binders produced by synthesising high-calcium fly ash (HCFA) and ground granulated blast furnace slag (GGBS) using sodium metasilicate anhydrous. Three test series were conducted in this study to investigate the effects of GGBS/binder, activator/binder and water/binder ratios on the fresh and hardened properties of the one-part synthesis AAB system. It was found that the SiO₂/Al₂O₃ molar ratio plays an important role in the attainment of compressive strength and limits the amounts of solid activators effective in contributing to the alkali-activation reaction process. The optimum SiO₂/Al₂O₃ molar ratio was found between 3.20 and 3.30. The test results revealed that the optimum proportion between HCFA and GGBS was discovered at a GGBS/binder ratio of 0.50. The optimum activator/binder ratio was between 0.08 and 0.12, and it is recommended that the water/binder ratio should not exceed 0.50. This study demonstrated the potential of the one-part synthesis method in the production of alkali-activated binder for practical structural applications.