To synthesize silica particles under mild conditions, we proposed a biomimetic synthesis method. The synthesis process was carried out based on a biphasic sol-gel synthesis method using TEOS (tetraethyl orthosilicate) as a silica source and PAH (polyallylamine) as a substitute for proteins of marine microorganisms for biosilicification. The function and activity of the PAH, used as a replacement for bioactive substances, were confirmed through comparisons between control experiments and designed experiments. The PAH exhibited the ability accelerate condensation with hydrolyzed TEOS in aqueous solutions. The PAH also exhibited high condensation activity in acidic and neutral conditions to produce silica particles. Moreover, PAH also created the nuclei of the silica particles, and the number of nuclei could be controlled by the concentration of PAH. In addition to exhibiting these unique capabilities, PAH did not generate any complexes or composites with the silica species. Depending on the synthesis conditions, the synthesized silica particles exhibited various shapes, such as sponge-like, self-assembled, irregular spherical and completely spherical shapes. The sizes of the primary particles were diverse, with a range from 10 nm to 50 nm. In particular, by adjusting the PAH concentration, it was possible to obtain nearly perfect spherical-shaped silica nanoparticles with uniform sizes, which has rarely been reported. Above all, using this paper, we can get closer to understanding the principles of silica formation using PAH as a replacement for the bioactive proteins of microorganisms. (C) 2017 Elsevier Inc. All rights reserved.