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Objectives. To assess heterogeneity in pandemic-period excess fatal overdoses in the United States, by location (state, county) and substance type. Methods. We used seasonal autoregressive integrated moving average (SARIMA) models to estimate counterfactual death counts in the scenario that no pandemic had occurred. Such estimates were subtracted from actual death counts to assess the magnitude of pandemic-period excess mortality between March 2020 and August 2021. Results. Nationwide, we estimated 25 668 (95% prediction interval [PI] = 2811, 48 524) excess overdose deaths. Specifically, 17 of 47 states and 197 of 592 counties analyzed had statistically significant excess overdose-related mortality. West Virginia, Louisiana, Tennessee, Kentucky, and New Mexico had the highest rates (20–37 per 100 000). Nationally, there were 5.7 (95% PI = 1.0, 10.4), 3.1 (95% PI = 2.1, 4.2), and 1.4 (95% PI = 0.5, 2.4) excess deaths per 100 000 involving synthetic opioids, psychostimulants, and alcohol, respectively. Conclusions. The steep increase in overdose-related mortality affected primarily the southern and western United States. We identified synthetic opioids and psychostimulants as the main contributors. Public Health Implications. Characterizing overdose-related excess mortality across locations and substance types is critical for optimal allocation of public health resources. (Am J Public Health. 2024;114(6):599–609. https://doi.org/10.2105/AJPH.2024.307618) [ABSTRACT FROM AUTHOR]