Abstract A nano-scale electrochemical sculpture (denoted here as NES) method has been developed to create TiO2 nanotube arrays on the surface of titanium sheets for improved bonding between titanium and carbon fiber reinforced epoxy composite laminates. For comparison, other surface treatments including anodization in NaOH, Na2SiO3, Na2C4H4O6 and EDTA electrolyte (denoted as NaTESi) and electrochemical etching in alkali solution (denoted as ALK) were carried out to investigate their effects on the surface morphology, wettability and the shear strength between titanium sheets and epoxy resin. The results from single-lap tests showed that the apparent shear strengths between titanium sheet and epoxy with NaTESi, ALK and optimized NES treatments have been improved by 37.2%, 53.9%, and 70.9%, respectively, in comparison with that of non-treated pristine samples. The samples in single-lap tests showed a mixture mode of cohesive and interfacial failures where the interfacial failure occurred at the epoxy/metal-oxide interface and the oxide films formed during the surface treatments remained intact. Utilizing the treated titanium sheets, fiber metal laminates (FMLs) were fabricated and their interlaminar shear strengths (ILSS) were found to increase by 43.5%, 56.1%, and 75.0%, respectively, compared to pristine samples, showing the promise of the nano-patterning technique.