This investigation highlights the effect of surface modification on polyimide by atmospheric pressure plasma treatment with different exposure time. Surface modification of polymer by plasma treatment essentially creates physical and chemical changes such as cross-linking and formation of free radicals. It also forms oxygen functionalization in the form of polar groups on polymer surface, hence improving the wetting and adhesion properties. It is observed that surface energy of the polymer increases with increasing exposure time of atmospheric pressure plasma. However, prolonged exposure time of plasma results in deterioration of the surface layer of polyimide resulting in degradation and embrittlement. Scanning electron microscopy and atomic force microscopy analysis reveal that there is a considerable morphological change on the polymer surface due to atmospheric pressure plasma treatment. X-ray photo electron spectroscopy analysis reveals that the oxygen functionalities of polymer surface increases significantly when polyimide is exposed to atmospheric pressure plasma. Untreated and atmospheric pressure plasma-treated polyimide sheet are adhesive bonded by employing polyimide adhesive as well as with titanium substrate. Due to surface modification of polyimide, it is observed that there is a significant increase in lap shear tensile strength, and therefore, this technology is highly acceptable for aviation and space applications.