Cuprous oxide materials are of growing interest for optoelectronic devices and were produced by several chemical and physical methods. Here, we report on the structural, optical, and electrical properties of CuxO thin films prepared by the pulsed laser deposition technique. The substrate temperature, as well as the oxygen partial pressure in the deposition chamber, were varied to monitor the copper to oxygen ratio within the deposited films. The growth conditions were carefully optimized to provide the highest conductivity and mobility. Thus, 100 nm thick cuprous oxide films (Cu2O) deposited at 750 °C exhibited a resistivity of 16 Ω∙cm, high mobility of 30 cm2/(V∙s), and a bandgap of around 2 eV. The film deposited at the optimized deposition parameters on Nb:STO (001) substrate with Au top electrode showed a photovoltaic response with an open circuit voltage of 0.56 V. These results path the way to efficient solar cells made with Cu2O films via the pulsed laser deposition technique.