Background: Associations between airborne particles and health outcomes have been documented worldwide; however, there is limited information regarding health effects associated with different particle sizes.Objectives: We explored the association between size-fractionated particle number concentrations (PNCs) and daily mortality in Shenyang, China.Methods: We collected daily data on cause-specific mortality and PNCs for particles measuring 0.25–10 μm in diameter between 1 December 2006 and 30 November 2008. We used quasi-Poisson regression generalized additive models to estimate associations between PNCs and mortality, and we used natural spline smoothing functions to adjust for time-varying covariates and long-term and seasonal trends.Results: Mean numbers of daily deaths were 67, 32, and 7 for all natural causes, cardiovascular diseases, and respiratory diseases, respectively. Interquartile range (IQR) increases in PNCs for particles measuring 0.25–0.50 μm were significantly associated with total and cardiovascular mortality, but not respiratory mortality. Effect estimates were larger for PNCs during the warm season than the cool season, and increased with decreasing particle size. IQR increases in PNCs of 0.25–0.28 μm, 0.35–0.40 μm, and 0.45–0.50 μm particles were associated with 2.41% (95% CI: 1.23, 3.58%), 1.31% (95% CI: 0.52, 2.09%), and 0.45% (95% CI: 0.04, 0.87%) higher total mortality, respectively. Associations were generally stable after adjustment for mass concentrations of ambient particles and gaseous pollutants.Conclusions: Our findings suggest that particles < 0.5 μm in diameter may be most responsible for adverse health effects of particulate air pollution and that adverse health effects may increase with decreasing particle size.Citation: Meng X, Ma Y, Chen R, Zhou Z, Chen B, Kan H. 2013. Size-fractionated particle number concentrations and daily mortality in a Chinese city. Environ Health Perspect 121:1174–1178; http://dx.doi.org/10.1289/ehp.1206398