In situ growth of ZnO quantum dots (QDs) on the surface of multiwalled carbon nanotubes (MWCNTs) was realized via a mild solution-process method, which resulted in an improvement in photoinduced charge separation and transport of carriers to the collecting electrode. The charge transfer efficiency was significantly increased by more than 90% due to the conjugation of ZnO QDs with MWCNTs, as confirmed by photoluminescence measurements. Ultraviolet photovoltaic cells based on the charge transfer at the ZnO QD-MWCNT heterostructures were fabricated, and their power conversion efficiency was measured to be above 1%.