Adhesive bonding has emerged as a promising technology for joining carbon fiber reinforced polymer (CFRP) structures in aircraft, offering advantages over traditional mechanical fastening such as weight reduction and uniform stress distribution. This study evaluates the effectiveness of innovative laser ablation and electrospinning surface treatments compared to the conventional peel-ply method for secondary bonding. Surface features and wetting behavior were characterized using scanning electron microscopy (SEM) and contact angle measurements, while mechanical performance was assessed via single lap shear tests. Results demonstrate that laser ablation (30 W power, 10 m/s speed) achieved the highest bond strength at 20.68 MPa, followed by electrospinning (18.20 MPa) using 10 wt% PA-66 nanofibers. Both advanced techniques significantly outperformed the peel-ply method, which yielded the lowest shear strength of 15.18 MPa. SEM analysis confirmed that laser treatment facilitated direct fiber exposure with minimal damage, while nanofibers provided enhanced physical interlocking. In conclusion, laser ablation proved to be the most effective technique for enhancing interfacial bonding in aerospace-grade CFRP structures, followed by electrospinning, offering a superior alternative to traditional surface preparation.