Coatings for functionalization of the surfaces are often used to trigger the interactions on the border of the non-viable materials to that of the vital biological tissue. Surface modifications influence many biological events, which include protein adsorption, cell adhesion and proliferation, and inflammatory response. Technique, which allows formation of nanometre scale coatings for medical implants and allows fulfilling the listed requirements, is the Layer-by-Layer polyelectrolyte coating procedure. It consists of alternately depositing of polyelectrolytes on charged surfaces. This is a self-assemble and self organisation process. leading to the formation thin layers (films) on the surfaces of the materials with a thickness of less than 1 µm and a precision of only few nanometres. The procedure is versatile and comparatively simple. The present article summarises the collected in the last years experience on using different building blocks (polyelectrolytes), different coating procedures and treatment of the materials to obtain coatings with desired properties. Examples of the use of the Layer-by-Layer coatings for cardiovascular stents, drug delivery systems of regulating adhesion of cells are presented.