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Background Dietary supplement use is prevalent in the general US population, but little is known regarding the driving reasons for their use among those with atherosclerotic cardiovascular disease (ASCVD). Methods and Results Data from the National Health and Nutrition Examination Survey (NHANES) from 2017 to March 2020 were used to identify adults with ASCVD. Supplement use was assessed by interviewers using label review, and surveys captured self‐reported reasons for use. Demographic, clinical, medication, and laboratory characteristics were compared between supplement users and nonusers. Among individuals with ASCVD in the National Health and Nutrition Examination Survey (n=965; mean age, 65 years; 56.1% men; 73.7% White individuals), 73.1% reported taking ≥1 dietary supplements, most commonly multivitamins (35.4%), vitamin D (30.8%), and fish oil (19.8%). Of those taking supplements, 47.3% report taking them under the advisement of a health professional. Nearly one fifth (17.9%) reported taking at least 1 supplement for “heart health,” most commonly fish oil (11.1%), followed by CoQ10 (4.2%) and resveratrol (1.5%). Supplement users were older (68 versus 62 years; P=0.003), included more women (45.8% versus 37.7%; P=0.17), were less likely to smoke (11.0% versus 36.4%; P