The focus of this survey is on survey data for adults aged 20 and above, covering nine survey cycles from 2001 to 2018. Additionally, the present study explored the correlation between vitamin D concentrations and both cardiovascular disease (CVD) and all-cause mortality. The objectives of this study were to evaluate the trend of changes in the serum 25(OH)D concentration changes in US adults during the survey period, the prevalence of vitamin D deficiency, and the current status of vitamin D dietary intake and supplementation. In-home health interviews were performed using meticulously designed questionnaires that gathered information on demographic details, socioeconomic conditions, dietary patterns, and overall health status. Health assessments were conducted in specially designed mobile centers. Survey data from 2001 to 2018 revealed a rise in serum 25(OH)D levels, from a weighted mean (95% CI) of 65.6 (63.8-67.4) nmol/L during 2001-2002 to 73.5 (70.4-76.5) nmol/L during 2017-2018, among US adults, while overall vitamin D deficiency rates remained stable (p = 0.152). Notably, in adults aged 20-39, 25(OH)D levels decreased (p = 0.002 for trend), and 25(OH)D deficiency increased (p = 0.003 for trend), especially among those with low incomes (deficiency >30%). Upon multivariable adjustment, an L-shaped relationship was found between serum 25(OH)D concentrations and both CVD and all-cause mortality (p < 0.001 for nonlinearity), as corroborated by sensitivity analyses. From 2001 to 2018, US adults experienced a significant increase in their serum 25(OH) D concentration. However, subgroups of individuals, including young adults and individuals with lower socioeconomic status, exhibited a heightened risk of 25(OH)D deficiency. Furthermore, an L-shaped relationship was found between 25(OH)D concentration and both all-cause and CVD mortality among US adults.