The inferior delamination resistance and out‐of‐plane performance of fiber metal laminates (FMLs) are of serious concerns. This work employs two modification methods, namely metal surface's chemical pre‐treatment and nano Al2O3 embedded interpenetrating polymer network (IPN) formation for improving the delamination resistance of aluminum and glass fiber‐reinforced polymer (GFRP) composite‐based FMLs. The synergetic effect of the two modification techniques resulted in high degrees of improvement in delamination resistance that were ~28% for critical strain energy release rate during mode‐I interlaminar fracture toughness (ILFT), that is (GIC) and ~37% for GIIC. Simultaneously, the flexural strength, tensile strength, and interlaminar shear strength improved by ~23%, ~17%, and ~24%, respectively. Scanning electron microscopy, atomic force microscopy, and surface energy measurement studies showed that the chemical pre‐treatment significantly influenced the surface morphology, surface roughness, and surface energy responses of aluminum, respectively. Fractographic study validated the effect of modification methods on the failure behavior under various testing modes.