Polyetheretherketone (PEEK) is widely used in dentistry owing to its exceptional properties, including its natural appearance; however, existing surface treatment methods for bonding PEEK have limitations. Autofocus laser cutters, known for their precise engraving and cutting capabilities, offer potential for surface treatment of PEEK; thus, the objective of this study was to investigate the creation of laser groove structures on PEEK to enhance its bonding capability with dental resin cement. A dental computer-aided design and manufacturing system was used to fabricate PEEK samples, and three groove patterns (circle, line, and grid) were generated on PEEK surfaces, with air-abrasion used as the control group. The surface characteristics, cell viability, and bond strength were evaluated, and the data were statistically analyzed using one-way analysis of variance and post hoc Tukey's tests (α = 0.05). Laser-treated PEEK exhibited a uniform texture with a groove depth of approximately 39.4 µm, hydrophobic properties with a contact angle exceeding 90°, a surface roughness of 7.3-12.4 µm, consistent topography, and comparable cell viability compared with untreated PEEK. Despite a decrease in bond strength after thermal cycling, no significant intergroup differences were observed, except for the line-shaped laser pattern. These findings indicate that the autofocus laser cutter effectively enhances the surface characteristics of PEEK by creating a uniform texture and grooves, showing promise in improving bonding properties, even considering the impact of thermal cycling effects.