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Particulate matter (PM) is an important metric for studying the health effects of household air pollution. There are limited data on PM exposure for children in homes that use biomass fuels, and no previous study has used direct measurement of personal exposure in children younger than 5 years of age. We estimated PM2.5 exposure for 1266 children in The Gambia by applying the cookhouse PM2.5–CO relationship to the child’s CO exposure. Using this indirect method, mean PM2.5 exposure for all subjects was 135 ± 38 μg/m3; 25% of children had exposures of 151 μg/m3 or higher. Indirectly estimated exposure was highest among children who lived in homes that used firewood (collected or purchased) as their main fuel (144 μg/m3) compared to those who used charcoal (85 μg/m3). To validate the indirect method, we also directly measured PM2.5 exposure on 31 children. Mean exposure for this validation data set was 65 ± 41 μg/m3 using actual measurement and 125 ± 54 μg/m3 using the indirect method based on simultaneously-measured CO exposure. The correlation coefficient between direct measurements and indirect estimates was 0.01. Children in The Gambia have relatively high PM2.5 exposure. There is a need for simple methods that can directly measure PM2.5 exposure in field studies.