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Introduction Smoking-related disparities continue to be a public health problem among American Indian/Alaska Native (AI/AN) population groups and data documenting the health burden of smoking in this population are sparse. The purpose of this study was to assess mortality attributable to cigarette smoking among AI/AN adults relative to non-Hispanic white adults (whites) by calculating and comparing smoking-attributable fractions and mortality. Methods Smoking-attributable fractions and mortality among AI/ANs ( n =1.63 million AI/ANs) and whites were calculated for people living in 637 Indian Health Service Contract Health Service Delivery Area counties in the U.S., from mortality data collected during 2001−2009. Differences in smoking-attributable mortality between AI/ANs and whites for five major causes of smoking-related deaths were examined. All data analyses were carried out in 2013−2014. Results Overall, from 2001 to 2009, age-adjusted death rates, smoking-attributable fractions, and smoking-attributable mortality for all-cause mortality were higher among AI/ANs than among whites for adult men and women aged ≥35 years. Smoking caused 21% of ischemic heart disease, 15% of other heart disease, and 17% of stroke deaths in AI/AN men, compared with 15%, 10%, and 9%, respectively, for white men. Among AI/AN women, smoking caused 18% of ischemic heart disease deaths, 13% of other heart diseases deaths, and 20% of stroke deaths, compared with 9%, 7%, and 10%, respectively, among white women. Conclusions These findings underscore the need for comprehensive tobacco control and prevention efforts that can effectively reach and impact the AI/AN population to prevent and reduce smoking.