Spin-coating is a widely employed technique for the fabrication of thin-film coatings over large areas with smooth and homogeneous surfaces. In recent years, research has extended the scope of spin-coating by developing methods involving the interface of the substrate and the deposited solution to obtain self-supported films, also called freestanding films. Thereby, such structures have been developed for a wide range of areas. Biomedical applications of spin-coated freestanding films include wound dressings, drug delivery, and biosensing. This review will discuss the fundamental physical and chemical processes governing the conventional spin-coating as well as the techniques to obtain freestanding films. Furthermore, developments within this field with a primary focus on tissue engineering applications will be reviewed.