Exposure to radioactivity inside homes potentially poses severe health risks which can be exacerbated by the interaction between radioactive particles and fine indoor particles; in particular, the presence of α particles are a key risk factor. Hence, in this study, particle radioactivity was concurrently measured in the family rooms and basements of 26 homes to assess its concentrations and identify its sources, both indoors and outdoors, across two seasons. The levels of radon, air ions, and particle radioactivity, which included short- and long-lived α-activity (SLA and LLA, respectively), varied greatly but were substantially higher in the basements. Also, particle radioactivity—as well as PM
2.5
and sulfur concentrations—were lower during the heating season. SLA was associated with radon, which was consistently of indoor origin, whereas LLA was more strongly related to the sulfur measured in indoor PM
2.5
, which is a proxy of outdoor infiltration. A regression model adjusted for sulfur and SLA also indicated a predominance of outdoor sources, likely due to the short residence time of indoor particles. Our results suggest that radiation in homes originates from both the decay of indoor radon and the infiltration of outdoor radioactivity.