High-volume fly ash mortar is considered a "green" material, a sustainable development solution for the construction industry, in which the fly ash replacement Portland cement content is over 50%. However, this material has the major disadvantage of slow strength development, especially at an early age, which limits its applicability. To overcome the above disadvantage, the individual or combined addition of lime Ca(OH)2, silica fume, and/or accelerating admixtures including sodium thiocyanate (NaSCN), diethanolamine (DEA), and glycerol (Gly), etc. have been interested recently. In this study, to enhance the early strength of mortars with fly ash content to replace 60÷80% of Portland cement, a three-component accelerating admixture of NaSCN, DEA, and Gly (2:1:0.5 by the mass) was used with different ratios of 0.21÷0.49 % by the total powder mass, combined with a reasonable amount of lime, silica fume supplement as presented in previous research. Experimental results showed that the optimal accelerating admixture content is 0.35% by weight of powder, combined with 6% silica fume and the additional amount of lime is 5%; 10%; and 15% corresponding to mortars using fly ash of 60%; 70% and 80%, respectively to improve early strength of mortars that are suitable for structural use (R3 ≥ 13MPa, 3 days old). In addition, the influence of the additives used on the initial setting time of high-volume fly ash mortars was also discussed.