Atmospheric particulate matter (PM) pollution is a major public health concern in Hong Kong. In this study, the spatiotemporal variations of health risks from ambient PM10 from seven air quality monitoring stations between 2000 and 2011 were analyzed. Positive matrix factorization (PMF) was adopted to identify major source categories of ambient PM10 and quantify their contributions. Afterwards, a point-estimated risk model was used to identify the inhalation cancer and non-cancer risks of PM10 sources. The long-term trends of the health risks from classified local and non-local sources were explored. Furthermore, the reason for the increase of health risks during high PM10 days was discussed. Results show that vehicle exhaust source was the dominant inhalation cancer risk (ICR) contributor (72%), whereas trace metals and vehicle exhaust sources contributed approximately 27% and 21% of PM10 inhalation non-cancer risk (INCR), respectively. The identified local sources accounted for approximately 80% of the ICR in Hong Kong, while contribution percentages of the non-local and local sources for INCR are comparable. The clear increase of ICR at high PM days was mainly attributed to the increase of contributions from coal combustion/biomass burning and secondary sulfate, while the increase of INCR at high PM days was attributed to the increase of contributions from the sources coal combustion/biomass burning, secondary nitrate, and trace metals. This study highlights the importance of health risk-based source apportionment in air quality management with protecting human health as the ultimate target.