The modification of a metal implant surface with a biomimetic coating of bone-like anisotropic and graded porosity structures to improve its biological anchorage with the surrounding bone tissue at implanting, is still a high challenge. In this paper, we present an innovative way of a gelatin (GEL) dip-coating on Ti-6Al-4V substrates of different square-net surface textures by the unidirectional deep-freezing process at simultaneous cross-linking using carbodiimide chemistry. Different concentrations of GEL solution were used to study the changes in morphology, density, and mechanical properties of the coatings. In addition, the surface free energy and polarity of Ti-6Al-4V substrate surfaces and GEL solutions have been evaluated to assess the wetting properties at the substrate interfaces, and to describe the adhesion of GEL macromolecules with their surfaces, being supported by mechanical pull-out testing. The results indicate that the coating’s morphology depends primarily on the Ti-6Al-4V substrate’s surface texture and second, on the concentration of GEL, which further influences their adhesion properties, orientation, morphological arrangement, as well as compression strength. The substrate with a 300 × 300 μm2 texture resulted in a highly adhered GEL coating with ≥80% porosity, interconnected and well-aligned pores of 75–200 μm, required to stimulate the bone ingrowth, mechanically and histologically.
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