Polyetheretherketone (PEEK) is known for its poor wettability and poor adhesive properties. Hence, for the creation of reliable high-strength structural adhesive bonded joints, surface treatment of PEEK is required. In this work high strength bondable PEEK surfaces were achieved through a vacuum-UV (VUV) treatment. Samples of amorphous and semi-crystalline PEEK films were exposed to different VUV radiation doses. Additionally oxygen low-pressure plasma (LPP) and untreated (as received) PEEK samples were investigated for comparison. Surfaces were characterized using x-ray photoelectron spectroscopy (XPS), contact angle measurements (CA), atomic force microscopy (AFM) and confocal laser scanning microscopy (CLSM). Tensile tests of the PEEK films were carried out, to investigate changes in the mechanical properties in the bulk of the PEEK films due to the VUV exposure. The adhesive bond strength of treated specimen was determined through two different test methods (tensile and shear). These strengths were compared to the created surface properties. A strong correlation between the contact angle and the creation of functional groups was observed. VUV radiation appears as a suitable pre-treatment method for PEEK, as adhesive bonds of high strength were achieved after 5 seconds. Additionally, the usage of a VUV excimer lamp is simple, cheap and easy for automation.