A dense, uniform and highly biologically active bone-like apatite layer can be formed in arbitrary thickness on any kind and shape of solid substrate surface by the following biomimetic method at ordinary temperature and pressure. First, a substrate is set in contact with particles of bioactive CaO SiO2 based glass soaked in a simulated body fluid (SBF) with inorganic ion concentrations nearly equal to those of human blood plasma. Second, the substrate is soaked in another solution with ion concentrations 1.5 times those of SBF (1.5 SBF). In the present study, organic polymer substrates treated with 5 M NaOH solution were subjected to the above mentioned biomimetic process. The induction periods for the apatite nucleation on polyethyleneterephthalate (PET), polymethylmethacrylate (PMMA), polyamide 6 (PA6), and polyethersulfone (PESF) substrates were reduced from 24 to 12 h with the NaOH treatment. The adhesive strength of the formed apatite layer were increased from 3.5 to 8.6 MPa, from 1.1 to 3.4 MPa, and from 0.6 to 5.3 MPa with the NaOH treatment, for PET, PMMA, and PA 6, respectively. It was assumed that highly polar groups, such as carboxyl and sulfinyl ones formed by the hydrolysis of an ester group on PET and PMMA and of an amide group on PA 6, or of a sulfonyl group on PESF with the NaOH treatment, attached a large number of hydrated silica dissolved from the glass particles, to accelerate the apatite nucleation, and also to form a strong bond with the apatite. The apatite-organic polymer composites thus obtained are expected to be useful as bone-repairing as well as soft tissue-repairing materials.