Children have higher polybrominated diphenyl ether (PBDE) body burdens than adults, which may be related to hand-to-mouth behavior. We investigate associations between children's behavior, including hand-to-mouth contacts, and markers of PBDE exposure. In addition, we investigate associations between characteristics of the home environment and exposure. Eighty-three children aged 12–36 months were recruited from North Carolina (2009–2010). Children provided blood and handwipes samples, which were analyzed for PBDEs. Parents completed questionnaires, providing demographic, behavioral, and environmental data. More active children had higher levels of PBDEs on their hands and in their bodies. For example, children who spent more time sleeping had lower exposures to PBDEs; each additional hour of sleep resulted in a 30% decrease in handwipe BDE-99 levels (P<0.001) and a 15% decrease in serum (P = 0.03). After accounting for handwipe PBDE levels, children who licked their fingers while eating had higher serum PBDEs. Other behaviors were not consistently associated with serum levels. Playing with plastic toys was associated with higher handwipe levels of PBDEs, while frequent vacuuming decreased handwipe PBDE levels. Characteristics of the home environment generally were not associated with serum PBDEs. Our results suggest that certain aspects of children's behavior and their environment impact exposure to PBDEs.