There are often bonding problems between acrylic resins and silicone. PEEK (polyetheretherketone), which is a high-performance polymer, has great potential for the implant, and fixed or removable prosthodontics. The aim of this study was to evaluate the effect of different surface treatments on PEEK to be bonded to maxillofacial silicone elastomers. A total of 48 specimens were fabricated from either PEEK or PMMA (Polymethylmethacrylate) (n = 8). PMMA specimens acted as a positive control group. PEEK specimens were divided into five study groups as surface treatments as control PEEK, silica-coating, plasma etching, grinding, or nano-second fiber laser. Surface topographies were evaluated by scanning electron microscopy (SEM). A platinum-primer was used on top of all specimens including control groups prior to silicone polymerization. The peel bond strength of the specimens to a platinum-type silicone elastomer was tested at a cross-head speed of 5 mm/min. The data were statistically analyzed (α = 0.05). The control PEEK group showed the highest bond strength (p< 0.05) among the groups. No statistical difference was found between control PEEK, grinding, or plasma etching groups (p> 0.05). The lowest bond strength was seen in the laser group, which was not statistically different from silica-coating (p> 0.05), and statistically different from control PEEK, grinding, or plasma groups (p< 0.05). Positive control PMMA specimens had statistically lower bond strength than either control PEEK or plasma etching groups (p< 0.05). All specimens exhibited adhesive failure after a peel test. The study results indicate that PEEK could serve as a potential alternative substructure for implant-retained silicone prostheses.