and superior properties, which are cost-effective [1] and found many applications in photocatalytic devices, [2,3] electronic devices, [4] solar cells, [5] sensors, [6] as well as biomedical implants. [7,8] As coatings on biomedical implants, TNT layers have been reported to affect the cellular behavior such as adhesion, [9] migration, [7] proliferation, [7,10] and differentiation. [11] Nevertheless, TNT coatings are normally deposited on pure titanium substrates rather than Ti alloys because TNT layers fabricated on Ti alloys are usually inhomogeneous. Most Ti alloys used in biomedical applications have a binary-phase α/β microstructure, [12] of which the α phase has a hexagonal close-packed crystallographic structure containing α-stabilizing elements like Al, O, and N, whereas the β phase with a body-centered cubic structure is enriched with β-stabilizing elements such as Nb, V, Mo, Ta, and Zr. [13] It is difficult to produce uniform nanotube arrays on multiple-phase substrates due to the diverse chemical reactivities of different phases. For example, one phase can be oxidized or etched preferentially by the electrolyte, [14] and hence the nanotube layers formed on Hexagonal TiO 2 nanotubes (TNTs) arrays are generally fabricated on Ti-based substrates for some biomedical purposes, but the TNT layers constructed on conventionally processed Ti alloys are usually inhomogeneous because the substrates typically contain both the α and β phases. In this work, high-pressure torsion (HPT) is applied to obtain a saturated single α-phase microstructure in Ti-6Al-4V alloys via strain-induced β phase dissolution. Homogeneous anodic TNT layers with three different morphologies, one-step nanoporous, one-step nanotubular, and two-step nanoporous structures, are electrochemically fabricated on the ultrafine-grained (UFG) Ti-6Al-4V alloy substrates after HPT processing, whereas the TNT layers prepared on coarsegrained substrates are normally inhomogeneous. More notably, the TNT layers show significantly improved adhesion strength to the UFG substrate as well as better corrosion resistance compared to those on the conventionally processed Ti-6Al-4V substrates. X-ray diffraction analysis, scanning electron microscopy in combination with electron backscatter diffraction, and transmission electron microscopy indicate that the improvement is due to a larger dislocation density in the UFG substrate as well as strain-induced β phase dissolution.