To improve the photoelectrochemical properties of TiO 2 /CdS composite nanorod electrodes, we developed a one-step quantum dot (QD) synthesis and assembly process based on pulsed laser deposition (PLD). An advantage of this method is that it does not involve ligand-exchange processing or wet chemical methods that might destabilize the QD attachment. By using PLD, CdS QDs were successfully grown on a dense array of TiO 2 nanorods, forming needle-like heterostructures whose photophysics depends on the laser pulse energy. The XRD results indicated that the products were composed of the tetragonal rutile, TiO 2 and hexagonal CdS. The TiO 2 /CdS heterostructures fabricated with this method are very stable and exhibit promising photoelectrochemical characteristics for photovoltaic applications. The best results are obtained for a PLD laser pulse energy of 300 mJ, which produces TiO 2 /CdS heterostructure nanorod electrodes that, when illuminated at AM 1.5 G, have a photocurrent density exceeding 4.7 mA cm−2 at 0 V versus a saturated calomel electrode. • Pulsed laser deposition (PLD) is a promising technique for fabricating quantum dot (QD) without ligand-exchange. • We grow CdS QDs on a dense array of TiO 2 nanorods, forming needle-like heterostructures. • TiO 2 /CdS(N) electrodes exhibit a stable photocurrent when illuminated with 100 mW cm−2 of simulated sunlight. [ABSTRACT FROM AUTHOR]