The aim of this study was the creation of a silicone hydrophilic surface prior to bonding. Modifications in wettability and adhesion properties of silicone were performed with an atmospheric plasma torch (APPT). Surface energy variations of the substrate, both pristine and APPT-treated, were evaluated through contact angle measurements, studying the hydrophobic recovery of the samples up to 24 hours of aging. Compositional and topographical changes induced by APPT and aging were studied by attenuated total multiple reflection mode infrared spectroscopy (ATR-FTIR), X-ray photoelectron spectroscopy (XPS), mechanical profilometry, scanning electron microscopy (SEM), and atomic force microscopy (AFM), respectively. Adhesion pull-off tests were performed on silicone-aluminium stud joints using three commercial adhesives, which were Sikaflex (R)-252, polyurethane-based, Loctite (R)-330, urethane methacrylate ester-based acrylic, and Terostat (R)-922, modified silicone. Although experimental data of all the bonding specimens led to an undesired adhesive failure, it was found that APPT-treated samples gave higher adhesive strength than the pristine ones, which was explained by the higher surface energy, thus more wettable material, after APPT. This effect remained stable for just 1 h, when the substrate began its hydrophobic recovery, reaching the original surface energy values after 24 h of aging.