Despite strong longitudinal associations between particle personal exposures and ambient concentrations, previous studies have found considerable inter-personal variability in these associations. Factors contributing to this inter-personal variability are important to identify in order to improve our ability to assess particulate exposures for individuals. This paper examines whether ambient, home outdoor and home indoor particle concentrations can be used as proxies of corresponding personal exposures. We explore the strength of the associations between personal, home indoor, home outdoor and central outdoor monitoring site (“ambient site”) concentrations of sulfate, fine particle mass (PM2.5) and elemental carbon (EC) by season and subject for 25 individuals living in the Boston, MA, USA area. Ambient sulfate concentrations accounted for approximately 70 to 80% of the variability in personal and indoor sulfate levels. Correlations between ambient and personal sulfate, however, varied by subject (0.1–1.0), with associations between personal and outdoor sulfate concentrations generally mirroring personal-ambient associations (median subject-specific correlations of 0.8 to 0.9). Ambient sulfate concentrations are good indicators of personal exposures for individuals living in the Boston area, even though their levels may differ from actual personal exposures. The strong associations for sulfate indicate that ambient concentrations and housing characteristics are the driving factors determining personal sulfate exposures. Ambient PM2.5 and EC concentrations were more weakly associated with corresponding personal and indoor levels, as compared to sulfate. For EC and PM2.5, local traffic, indoor sources and/or personal activities can significantly weaken associations with ambient concentrations. Infiltration was shown to impact the ability of ambient concentrations to reflect exposures with higher exposures to particles from ambient sources during summer. In contrast in the winter, lower infiltration can result in a greater contribution of indoor sources to PM2.5 and EC exposures. Placing EC monitors closer to participants' homes may reduce exposure error in epidemiological studies of traffic-related particles, but this reduction in exposure error may be greater in winter than summer. It should be noted that approximately 20% of the EC data were below the field limit of detection, making it difficult to determine if the weaker associations with the central site for EC were merely a result of methodological limitations.