The use of the thermal power plant ashes including fly ash (FA) and bottom ash (BA) for producing unfired building bricks (UBB) using sodium hydroxide (NaOH) solution as an alkaline activator was investigated. A low applied forming pressure of 0.5 MPa and various NaOH concentrations of 5, 8, 10, and 12 M were used for the preparation of brick samples with different solution-to-binder (S/B) ratios of 0.35 and 0.40. The bricks were subjected to various test programs with reflecting the effect of both NaOH concentrations and S/B ratios on the brick’s properties. The compressive strength, unit weight, ultrasonic pulse velocity, and thermal conductivity of bricks increased with increasing NaOH concentration, whereas the contrary trend was found with increasing S/B ratio. Also, the water absorption of bricks was observed to reduce with increasing NaOH concentration and decreasing S/B ratio. As the results, the combined utilization of both low forming pressure and coal power plant ashes can produce the UBBs with low unit weight, low heat conductivity, and acceptable strength and water absorption rate as stipulated by TCVN 6477-2016. Furthermore, the outcomes of chemical analysis and microstructure observation also demonstrate that a high concentration of the NaOH promoted the geopolymerization process. Notably, the use of NaOH solution of either 10 M or above is recommended for the production of UBBs, which are classified as grade M5.0 or higher.