<p>In this study, to improve the bonding strength and interlaminar fracture toughness of hot-pressed joints fabricated using aluminum alloys and carbon fiber-reinforced thermoplastic laminates (polyetheretherketone as the matrix), several pretreatment strategies were implemented to modify the aluminum surface. Specifically, we evaluated the optimal conditions for silane coupling treatment and determined the effects of surface microstructuring on the bonding strength and interlaminar fracture toughness. The experimental results suggested that reducing the hydrolysis time of the amino-silane coupling agent reduces the reaction between silanols and improves the bonding strength. In addition, the bonding strength of specimens pretreated using a pulse wave laser to make grooved structures on the aluminum alloy surface was up to 1.97 times higher than specimens without grooved structures. The interlaminar fracture toughness of the specimen with a grooved structure on the surface of the aluminium alloy was approximately 2.8 times that of the specimen without a structure, and for the bonded specimen with a nano-structure introduced by anodisation and etching, it was approximately 2.0 times. Our findings also help clarify the mechanisms behind these improvements. By refining the hydrolysis conditions of the silane coupling agent, we strengthened the chemical bonding at the interface. Furthermore, the additional micro and nanoscale structures enhanced mechanical interlocking and promoted plastic deformation during crack propagation. Ultimately, these effects partially overcome the inherent trade-off between strength and toughness, supporting the development of advanced applications.</p>