The weak adhesion of anodic TiO2 nanotube arrays (TNTAs) to the underlying Ti substrate compromises many promising applications. In this work, a compact oxide layer between TNTAs and Ti substrate is introduced by employing an additional anodization in a fluoride-free electrolyte. The additional anodization results in an about 200 nm thick compact layer near the nanotube bottoms. Scratch test demonstrates that the critical load of TNTAs with the compact oxide layer is a more than threefold increase in comparison with those without the compact layer. Moreover, this facile method can also improve the photoactivity and supercapacitor performances of TNTAs markedly.