This work reports the growth of stable TiO2 nanotube arrays on flexible Kapton substrates by electrochemical anodization of a sputtered Ti (titanium) film. Although such nanotubes are conventionally fabricated on Ti foils, obtaining these on polymer-based flexible substrates remained a challenge because of higher annealing temperature not compatible with thermal stability of the substrates. Here, we demonstrate the fabrication of TiO2 nanotubes (1.5 μm long and 80 nm diameter) by anodization of the Ti film deposited using the RF sputtering technique at two different substrate temperatures (room temperature and 300 °C). Nanoindentation and nanoscratch techniques reveal better adhesion of the Ti film with an underlying Kapton substrate for 300 °C deposition temperature. Such investigations reveal a more than twofold enhancement of the "rear pileup"for the Ti film deposited at elevated temperature compared to that at room temperature. The amorphous TiO2 nanotubes are crystallized at 220 °C for 3 h using a solvothermal technique that allows crystallization at temperatures much lower than the annealing temperature. Application of these nanotubes for photo-electrochemical water splitting reveals a photocurrent density of 18 μA/cm2 under AM 1.5 G conditions. Furthermore, the charge density and flat band potential (VFB) are calculated from Mott-Schottky analysis, showing features comparable to the TiO2 nanotubes on the Ti foil crystallized through thermal annealing. The present work establishes a scalable approach for developing TiO2 nanotube arrays on the flexible substrate and its use for photo-electrochemical solar energy conversion. © 2020 American Chemical Society. All rights reserved.