Calcium phosphate (CaP)-based thin layers and nanospheres have various potential biomedical applications. This paper describes the laser-assisted fabrication of CaP-based thin layers and nanospheres, with a focus on a new physicochemical process developed by us. This process is conducted under normal pressure and temperature in supersaturated CaP solutions using pulsed laser irradiation. Owing to the light-mediated solid-liquid interactions, this process enables the simple and rapid fabrication of CaPs. In addition, the physicochemical and biological properties of CaPs can be controlled by manipulating the processing conditions. Our physicochemical process provides a new tool for fabricating CaP-based thin layers and nanospheres for biomedical applications.