This study aimed to evaluate the effects of different surface modification methods on the surface roughness, contact angle, and bond strength of composite-veneer materials of polyether-ether-ketone (PEEK). Fifty-five specimens (n = 11) with a size of 7 × 7 × 2mm were cut out from PEEK discs. The specimens were divided into five groups with different surface treatments: no treatment (NO) (control group), sulfuric acid (SA), plasma (P), femtosecond laser (FS), and Nd-YAG laser (NY). After the surface treatments, the specimens were checked for roughness, contact angle, and bond strength of the composite-veneer material. Data were analyzed with the Welch test for roughness, contact angle, and bond strength parameters. Individual Pearson correlation tests were executed for all surface treatment groups to determine any significant correlations among roughness, contact angle, and bond strength parameters (P < .001). Roughness, contact angle, and bond strength values were affected by surface modification methods (P < .001). In comparison to the control group, NY and FS treatments increased the surface roughness and bond strength; they also provided bond strength values comparable to the SA group. When the relationship between the variables was examined, no correlation was seen between roughness, contact angle, and bond strength values for the NY, SA, and control groups (P > .05); however, significant correlations were determined between the contact angle and surface roughness values for the P and FS groups (P < .05). Femtosecond and Nd-YAG laser treatments are viable surface modification alternatives to the sulfuric acid treatment for the PEEK material.