Objectives The main purpose of this study is to evaluate the efficacy of polyetheretherketone (PEEK) as a material for prefabricated crown restorations in pediatric dentistry, particularly for restoring primary tooth structure defects. Materials and methods This study analyzed the effects of three surface treatment modalities on PEEK's surface morphology, wettability (as measured by contact angle), and shear bond strength. These treatments included alumina (AlO) sandblasting alone, and in conjunction with a 98% sulfuric acid pretreatment. Subsequently, an evaluation was conducted to assess the compressive and fatigue properties of self-fabricated PEEK preformed crowns, preformed metal crowns, and preformed zirconia crowns. Results AlO sandblasting followed by sulfuric acid pretreatment significantly enhanced the bond strength of PEEK. PEEK crowns, when compared with stainless steel and zirconia crowns, showed similar compressive and fatigue strengths to zirconia crowns but lower than metal alternatives. Additionally, PEEK crowns required less extensive modification of dental abutments compared to zirconia crowns. Conclusions The study concludes that PEEK prefabricated crown, especially after alumina (AlO) sandblasting in conjunction with a 98% sulfuric acid pretreatment, exhibits improved bond strength and favorable material characteristics for use in pediatric dental restorations. Clinical relevance The findings highlight the potential of PEEK prefabricated crowns in pediatric dentistry as a viable option for the aesthetic restoration of primary teeth, offering benefits over traditional materials like stainless steel and zirconia in terms of preferable compressive and fatigue strengths and ideal reduction of dental abutments.