A one-step sol-gel method was developed to synthesize nonspherical organosilica particles with tunable morphology. The morphology of organosilica particles can be tuned from spherical to golf ball-like or bowl-like through varying the molar ratio of tetraethoxysilane (TEOS) to vinyltrimethoxysilane (VTMS) in the precursors. The morphology and interior structure of the organosilica particles were observed by scanning electron microscopy (SEM) and transmission electron microscopy (TEM), respectively. The effect of ammonia concentration on the morphology of organosilica particles was investigated. The growth process of golf ball-like and bowl-like particles was tracked by SEM in detail, and the formation mechanism of nonspherical organosilica particles was also proposed.