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The electrical signals generated by an electromechanical coupling mechanism in biomaterials have significant potential applications in the field of biomedical engineering. For example, the piezoelectric- or flexoelectric-induced electrical signals in bone biomaterials play an important role in facilitating self-repair, remodeling, and reshaping processes. Polyetheretherketone (PEEK) has been found to possess excellent mechanical properties and biocompatibility with bone, making it an outstanding choice as an implantable polymer material. It is particularly important to investigate the electromechanical response performance of PEEK materials. In this study, we experimentally examine the flexoelectricity of PEEK and evaluate its effective out-of-plane direct and converse flexoelectric coefficients. Using the piezoresponse force microscopy module of atomic force microscopy, we observe a clear converse flexoelectric effect in a PEEK disk-shaped sample. The effective out-of-plane converse flexoelectric coefficient of the PEEK disk-shaped sample is about μ 3333 eff = 0.21 ± 0.02 nN / V. The effective out-of-plane direct flexoelectric coefficient, determined through the bending experiment of a PEEK cantilever, is f 3113 eff = 17.61 nC/m, which is larger than that of polyvinylidene fluoride and is nearly two orders of magnitude superior over other biomaterials such as bone and hydroxyapatite. This indicates that PEEK materials have even greater potential for development and research in biomedical engineering applications such as intervertebral fusion, bone joint replacement, bone rehabilitation and regeneration, etc. [ABSTRACT FROM AUTHOR]