Dense and well-aligned arrays of TiO2 nanotubes extending from various substrates are successfully fabricated via a new liquid-phase atomic layer deposition (LALD) in nanoporous anodic alumina (AAO) templates followed by alumina dissolution. The facile and versatile process circumvents the need for vacuum conditions critical in traditional gas-phase ALD and yet confers ALD-like deposition rates of 1.6–2.2 Å cycle−1, rendering smooth conformal nanotube walls that surpass those achievable by sol–gel and Ti-anodizing techniques. The nanotube dimensions can be tuned, with most robust structures being 150–400 nm tall, 60–70 nm in diameter with 5–20 nm thick walls. The viability of TiO2 nanotube arrays deposited on indium tin oxide (ITO)–glass electrodes for application in model hybrid poly(3-hexylthiophene) (P3HT):TiO2 solar cells is studied. The results achieved provide platforms and research directions for further advancements.