Despite the widespread availability of COVID-19 vaccines, the United States has a depressed rate of vaccination relative to similar countries. Understanding the psychology of vaccine refusal, particularly the possible sources of variation in vaccine resistance across U.S. subpopulations, can aid in designing effective intervention strategies to increase vaccination across different regions. Here, we demonstrate that county-level moral values (i.e., Care, Fairness, Loyalty, Authority, and Purity) are associated with COVID-19 vaccination rates across 3,106 counties in the contiguous United States. Specifically, in line with our hypothesis, we find that fewer people are vaccinated in counties whose residents prioritize moral concerns about bodily and spiritual purity. Further, we find that stronger endorsements of concerns about Fairness and Loyalty to the group predict higher vaccination rates. These associations are robust after adjusting for structural barriers to vaccination, the demographic makeup of the counties, and their residents' political voting behavior. Our findings have implications for health communication, intervention strategies based on targeted messaging, and our fundamental understanding of the moral psychology of vaccination hesitancy and behavior. (PsycInfo Database Record (c) 2022 APA, all rights reserved).