This chapter provides an overview of recent advances in the field of laser-based synthesis of biopolymer thin films for biomedical applications. The introduction addresses the importance of biopolymer thin films with respect to several applications like tissue engineering, cell instructive environments, and drug delivery systems. The next section is devoted to applications of the fabrication of organic and hybrid organic-inorganic coatings. Matrix-assisted pulsed laser evaporation (MAPLE) and Combinatorial-MAPLE are introduced and compared with other conventional methods of thin films assembling on solid substrates. Advantages and limitations of the methods are pointed out by focusing on the delicate transfer of bio-macromolecules, preservation of properties and on the prospect of combinatorial libraries' synthesis in a single-step process. The following section provides a brief description of fundamental processes involved in the molecular transfer of delicate materials by MAPLE. Then, the chapter focuses on the laser synthesis of two polysaccharide thin films, namely Dextran doped with iron oxide nanoparticles and Levan, followed by an overview on the MAPLE synthesis of other biopolymers. The chapter ends with summary and perspectives of this fast-expanding research field, and a rich bibliographic database.