In the production of artificial bone and tooth implants, coating of the surfaces of hard, but bioinert materials (metals, polymers) with calcium phosphate crystals has been used to improve bioactivity and facilitate osteointegration. Recently low temperature methods, involving precipitation from aqueous solutions (biomimetic precipitation) including coprecipitation of specific organic macromolecules (growth hormones, enzymes, proteins) have been developed. In this paper an alternative approach is presented, which consists in first laying down a matrix consisting of polyelectrolyte multilayers (PE MLs) alternating with layers of amorphous calcium phosphate (ACP) particles and subsequently growing calcium phosphate crystals upon/within the multilayers. This attractive approach leads to the formation of a new class of true organic-inorganic nanocomposite coatings. In a previous communication we have shown preliminary results, which point to the feasibility of this approach . Here we describe in detail the design, synthesis and characteristics of the thus obtained nanocomposite coatings.