Background and Purpose—Acute exposure to particulate matter with aerodynamic diameter <2.5 μm (PM2.5) is associated with acute cardiovascular and cerebrovascular mortality. The aim of this study was to evaluate these associations with specific causes of cardiovascular and cerebrovascular mortality in Mexico City.Methods—We obtained daily mortality records for Mexico City from 2004 to 2013 for cardiovascular and cerebrovascular causes in people ≥25 and ≥65 years old. Exposure to PM2.5 was assessed with daily estimates from a new hybrid spatiotemporal model using satellite measurements of aerosol optical depth PM2.5 and compared to ground level PM2.5 measurements with missing data estimated with generalized additive models PM2.5. We fitted Poisson regression models with distributed lags for all mortality outcomes.Results—An increase of 10 µg/m3 in aerosol optical depth PM2.5 was associated with increased cardiovascular (1.22%; 95% confidence interval, 0.17–2.28) and cerebrovascular mortality (3.43%; 95% confidence interval, 0.10–6.28) for lag days 0 to 1 (lag 0–1). Stronger effects were identified for hemorrhagic stroke and people ≥65 years. Associations were slightly smaller using generalized additive models PM2.5.Conclusions—These results support the evidence that acute exposure to PM2.5 is associated with increased risk of specific cardiovascular and cerebrovascular mortality causes.