Background/Objectives: Vitamin D deficiency is a public health concern worldwide. Maintaining vitamin D sufficiency during growth periods is essential. We aimed to determine the prevalence and predictors of vitamin D deficiency in Australian adolescents and young adults. Subject/Methods: We used data from adolescents (12–17 years, n = 692) and young adults (18–24 years, n = 400) who participated in the nationally representative 2011–2013 Australian Health Survey. Serum 25-hydroxyvitamin D concentrations were measured using a method certified to international standards, with prevalence reported for 125 nmol/L. Independent predictors of vitamin D deficiency were determined using a survey-weighted Poisson regression model. Results: Overall, 17% of adolescents and 32% of young adults were vitamin D deficient. In models adjusted for sex, age, region of birth, socioeconomic status, BMI and season (and education, smoking status and physical activity in young adults only), the prevalence ratio (PR) for vitamin D deficiency was more than double in participants born outside Australia (adolescents: PR 2.46; 95% confidence interval (CI) = 1.59, 3.81; young adults: PR 2.12; 95% CI = 1.46, 3.07), and also varied by season (adolescents: spring vs summer PR 2.47; 95% CI = 1.22, 5.01 and winter vs summer PR 2.01; 95% CI = 1.03, 3.92; young adults: winter vs summer; PR 3.32; 95% CI = 1.69, 6.53). Other predictors of vitamin D deficiency were overweight compared with healthy weight (adolescents) and lower physical activity (young adults). Conclusions: Strategies based on safe sun exposure and dietary approaches are needed to achieve and maintain adequate vitamin D status, particularly in young adults.