The issues associated with the fabrication of nano-silica (NS) mineral powder, such as high cost and agglomeration, can be effectively mitigated by using a precursor solution of NS as the external mixture of cement-based materials. Based on the liquid-phase preparation of NS mineral powder, its preparation technology was thoroughly investigated herein. The precursor solution of NS was synthesized using acid media (HCL, HNO3, HBO3, HCOOH, CH3COOH)—the acetic acid concentration was 1%~15%—and siliceous materials. (The concentration of sodium silicate was 20%~38%.) In addition, the pH value (pH4~pH8) of the precursor solution was measured using a pH detector. The indexes of NS, such as precipitation time, morphology, and distribution, were observed to formulate a preparation technique for the precursor solution of NS that possessed the best results for the precipitation of nanoparticles. From the acquired results, it was demonstrated that acetic acid solution (concentration ≤ 3%) and sodium silicate solution (concentration ≤ 25%) were mixed into a solution with pH = 6, which was the optimum mixing ratio for the precursor solution of NS. The prepared precursor solution of NS was also added to the Ca(OH)2 saturated solution, and the precursor solution became active from a stable state. Then, NS particles were precipitated in an alkaline solution and reacted with Ca(OH)2 to form calcium silicate gel, which made the solution increasingly turbid and generated many visible and uniformed flocculating substances. With time, gels were continuously produced, which then turn white. Similarly, NS particles can be precipitated when the precursor solution is added to cement paste, which reacts with the Ca(OH)2 to generate CSH gel and improve the compactness of the cement paste.