Due to excellent specific mechanical and physical properties, titanium-based fibre metal laminates (FML) have attracted increasing attention in marine and defense for improved impact protection. Metal and composite interface (MCI) plays a pivotal role to determine the failure mode of FML. Surface treatment of metal is commonly carried out to improve the MCI properties. In this study, two different electrochemical surface treatments, anodization and micro-arc oxidation (MAO) were adopted. The tunable hierarchical structure observed after multiple physical and chemical surface treating processes, i.e., sandblasting, anodization, etching,and annealing on Ti6Al4V. In comparison single step MAO treatment shows more pores and craters on the surface with increasing anodic voltage. The results from lap shear experiment show that the adhesive strength between Elium® resin and titanium adherend by single-step MAO treatment has been improved compared to that by multi-step anodization. By increasing the anodic voltage of MAO treatment to 600V, the highest shear strength of 18.4MPa is achieved.