Understanding the long-term behavior of rainfall and potential evapotranspiration (PET) over watersheds is crucial for the monitoring of hydrometeorological processes and climate change at the regional scale. The São Francisco watershed (SFW) in Brazil is an important hydrological system that transports water from humid regions throughout the Brazilian semiarid region. However, long-term, gapless meteorological data with good spatial coverage in the region are not available. Thus, gridded datasets, such as the Climate Research Unit TimeSeries (CRU TS), can be used as alternative sources of information, if carefully validated beforehand. The objective of this study was to assess CRU TS (v4.02) rainfall and PET data over the SFW, and to evaluate their long-term (1942–2016) climatological aspects. Point-based measurements retrieved from rain gauges and meteorological stations of national agencies were used for validation. Overall, rainfall and PET gridded data correlated well with point-based observations (r = 0.87 and r = 0.89), with a poorer performance in the lower (semiarid) portion of the SFW (r ranging from 0.50 to 0.70 in individual stations). Increasing PET trends throughout the entire SFW and decreasing rainfall trends in areas surrounding the semiarid SFW were detected in both gridded (smoother slopes) and observational (steeper slopes) datasets. This study provides users with prior information on the accuracy of long-term CRU TS rainfall and PET estimates over the SFW.