Recent studies have found associations between particulate air pollution and total and adult mortality. The relationship between particulate air pollution and mortality among infants has not been examined in the United States. This study evaluates the relationship between postneonatal infant mortality and particulate matter in the United States. Our study involved analysis of cohorts consisting of approximately 4 million infants born between 1989 and 1991 in states that report relevant covariates; this included 86 metropolitan statistical areas (MSAs) in the United States. Data from the National Center for Health Statistics-linked birth/infant death records were combined at the MSA level with measurements of particulate matter 10 microns or less (PM10) from the EPA's Aerometric Database. Infants were categorized as having high, medium, or low exposures based on tertiles of PM10. Total and cause-specific postneonatal mortality rates were examined using logistic regression to control for demographic and environmental factors. Overall postneonatal mortality rates were 3.1 among infants with low PM10 exposures, 3.5 among infants with medium PM10 exposures, and 3.7 among highly exposed infants. After adjustment for other covariates, the odds ratio (OR) and 95% confidence intervals (CI) for total postneonatal mortality for the high exposure versus the low exposure group was 1.10 (1.04, 1.16). In normal birth weight infants, high PM10 exposure was associated with respiratory causes [OR = 1.40, (1.05, 1.85)] and sudden infant death syndrome [OR = 1.26, (1.14, 1.39)]. For low birth weight babies, high PM10 exposure was associated, but not significantly, with mortality from respiratory causes [OR = 1.18, (0.86, 1.61)]. This study suggests that particulate matter is associated with risk of postneonatal mortality. Continued attention should be paid to air quality to ensure optimal health of infants in the United States.