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Polyetheretherketone (PEEK) is a highly biocompatible polymer widely used in medicine as an implant production material. In this article, the PEEK surface was characterized in terms of its wettabillity properties after the physicochemical modifications by treatment with the low‐temperature air plasma and covering with the Langmuir–Blodgett (LB) monolayers of polypeptide (cyclosporine A, CsA) and/or phospholipid (1,2‐dipalmitoyl‐sn‐glycero‐3‐phosphocholine, DPPC). The LB deposition was preceded by the analysis of miscibility and morphology of monolayers at the air/water interface by means of the Langmuir technique and Brewster angle microscopy (BAM). Then, wettability of the polymer‐supported films was evaluated by the contact angle measurements of three probe liquids of different characters (two polar—water and formamide, one apolar—diiodomethane). The measured contact angles allowed for determination of the surface free energy and its components based on the Lifshitz‐van der Waals/acid–base (LWAB) approach. Some relations between the kind and magnitude of interactions within the model membranes on the water subphase and those of the PEEK‐supported membranes with the liquids were found out. The results allowed obtaining the interesting models of biological coatings with potential applications. [ABSTRACT FROM AUTHOR]