Oxytocin (OT) is a neuropeptide critically involved in social cognition and behavior. Intranasal administration of OT has modulatory effects on both brain and behavior, with potential for therapeutic benefit, especially in individuals with deficits in socioemotional functions. Intranasal OT effects have been well-investigated in younger adults as well as in a variety of clinical populations (e.g., autism, schizophrenia), but there is comparatively less investigation of its function in older adults. To foster more research on OT and aging, the following dataset was made publicly available, which includes data from generally healthy younger (n = 52; aged 18-31 years; 48% female) and older adults (n = 54; aged 63-81 years; 56% female) who self-administered a single dose (24 international units) of either intranasal OT or a placebo (with identical ingredients as the OT spray but without the synthetic OT; IND 100,860; NCT01823146). The study adopted a randomized, double-blind, between-subject design. The dataset consists of anatomical and functional resting-state neuroimaging scans acquired after nasal spray administration as well as study-specific phenotypic and demographic data. This dataset using both OT administration and neuroimaging is unique in its size and inclusion of both younger and older adults as well as women and men. This data has resulted in published work on OT modulation of cognition, behavior, and neural activation/connectivity. Open access to this data will provide the scientific community with the opportunity to investigate individual differences in the neurocognitive effects of single-dose OT in younger and older adults.