There is an increasing interest in plant-based diets and higher levels of plant proteins due to rising concerns around health and environmental sustainability issues. We determined the effects of increasing quartiles of plant protein in the diet on nutrient adequacy using a large nationally representative observational dataset. Twenty-four-hour dietary-recall data from NHANES 2013–2018 from 19,493 participants aged 9+ years were used to assess nutrient intakes. Nutritional adequacy was assessed by estimating the percentage of the population with intakes below the EAR or above the AI. A quartile trend was assessed using regression and the significance was set at Pquartile trend < 0.05. With increasing quartiles of plant protein, the adequacy decreased for calcium, potassium, and vitamin D and increased for copper and magnesium for adolescents. Among the adults aged 19–50 years, the adequacy decreased for protein, choline, selenium, vitamin B12, and zinc and increased for copper, folate, iron, magnesium, thiamin, and vitamin C with increasing quartiles of plant protein. The adequacy for calcium, vitamin A, and zinc decreased and it increased for copper, folate, magnesium, thiamin, and vitamin C with increasing quartiles of plant protein among adults aged 51+ years. The results indicate that diets of mixed protein sources (from both animals and plants) are the most nutritionally adequate.