A facile and one-pot strategy for the preparation of novel diamino-functionalized hollow siliceous spheres (DAF-HSS) is suggested. Field-emission scanning electron microscopy (FE-SEM) images of DAF-HSS showed a monodispersed hollow sphere morphology. Also, TEM images revealed that the DAF-HSS has a porous structure with parallel semi-long-range channels. DAF-HSS material was used as an adsorbent for the removal of hazardous monocationic dyes in aqueous solution. Neutral red (NR) and crystal violet (CV) were selected as model compounds. Isotherm and kinetic studies were carried out and their different linear forms were applied and compared. The equilibrium data fitted better with the Langmuir model.