Background: A balanced diet is an important lifestyle component and has been associated with a reduced risk of chronic diseases. Objectives: To assess dietary intake of adult residents in Luxembourg taking part in two population-based cross-sectional studies (ORISCAV-LUX, 2007–2008 and ORISCAV-LUX 2, 2016–2017). Methods: Dietary intake of the study participants (1242 in 2007/08 and 1326 in 2016/17), 25–69 years old, were evaluated using food-frequency questionnaires (134 items in 2007/2008 and 174 items in 2016/2017) according to the French ANSES-CIQUAL food composition database. Both food-group- and nutrient-based analyses were conducted. Results: Dietary patterns in ORISCAV-LUX 2, 2016–2017, were characterized by an increase in the estimated marginal means (EMM) of the intake of energy, total fat, saturated fatty acids, alcohol, and decreased EMM of total carbohydrates, magnesium, and calcium compared to 2007/08. We also observed an increased EMM of the intake of protein-rich food items and ready-to-eat foods/fast foods, together with a decreased intake of grains, dairy products, and vegetables (all p-values <0.05, linear mixed models). The intake of most micronutrients was stable or slightly increased in ORISCAV-LUX 2 vs. ORISCAV-LUX, except for the drop in magnesium and calcium, and generally met recommendations, in particular, EFSA population reference intakes (PRI), except for vitamin D. Conclusions: Though most micronutrient recommendations were met, nutrient consumption in terms of high energy, total fat, and sodium, as well as low carbohydrates, were not aligned with recommendations for balanced eating.