Organotalcs, in which organic moieties are covalently bonded to Si atoms belonging to the tetrahedral sheets, are usually prepared by a sol-gel process starting from ethanolic solution of Mg nitrate, organo-alcoxysilanes, and aqueous sodium hydroxide solution. In this case, gypsum-like particles are obtained. In this work, evaporation-induced self-assembly within aerosols was used for the first time in order to prepare organotalc spheres. These hybrid lamellar materials can be used as environmental barriers, as polymer fillers, and as catalytic supports. Using octyltriethoxysilane as a source of Si, spherical particles with sizes ranging from 20 nm to 1 µm are obtained. X-ray diffraction and transmission electron microscopy images show that the d001 value equals 2.8 nm meaning that, in this case, organic moities are either alternatively distributed or identically tilted in the interlayer space. Compared to the classical synthesis at room temperature or in autoclaves, and besides being a continuous process, the reaction time is reduced to several minutes instead of hours. Homogeneous forms are obtained by aerosol whereas irregular shapes are obtained in the classical synthesis.