Narrow band gap semiconductors like cadmium sulfide (CdS) are being applied as an agent to reduce the band gap of metal oxide semiconductors like titanium dioxide (TiO2). In order to obtain a TiO2/CdS nanocomposite with reduced electron-hole recombination and improved stability, we coupled 10%, 20%, and 40% by weight of CdS with TiO2 in this work using pulsed laser ablation in liquid technique. Here, 532 nm wavelength generated from neodymium-doped yttrium aluminum garnet laser was directed into the TiO2/CdS mixture prepared in a colloid form to produce the TiO2/CdS nanocomposites. The effect of the CdS concentration on the performance of the obtained nanocomposite in a dye-sensitized solar cell and photocatalytic degradation of methyl orange in water was studied in detail. However, the nanocomposite with 10% percentage weight of CdS in anatase TiO2 showed the best performance as compared with pure TiO2, and the photoconversion efficiency of the dye-sensitized solar cell was improved from 0.6% to 4.3%, while the percentage of methyl orange degraded was enhanced from 58% to 82% after 36 min irradiation using ultraviolet-visible light. This improvement in photovoltaic and photodegradation properties is due to limited electron hole recombination rate, higher conduction of charge carriers, their longer lifetime during the photocatalytic process, improved ultraviolet-visible light activity, reduced photocorrosion, and improved pore size. Copyright (c) 2017 John Wiley & Sons, Ltd. Nanocomposite of TiO2 and CdS was prepared with pulsed laser ablation in liquid to enhance charge transfer for solar energy harvesting applications.