Children are encouraged to eat a specific amount of fruits and vegetables to optimize health. The purpose of this study was to assess whether consumption of a variety of fruits and vegetables, respectively, was associated with a greater diet quality among preschool-aged children. Analyses were performed using a cross-sectional, nationally representative sample of US children. Dietary intakes from 24-h dietary recalls of two-five year old children (n = 2595) in 2005–2010 NHANES were examined. Diet quality was evaluated using MyPlate equivalents and the Healthy Eating Index 2010 (HEI-2010). Variety categories were determined based on children's fruit, fruit juice, and vegetable consumption on the recalled day. Differences in diet quality were examined using t-tests. Variety of fruits and vegetables was linked to higher overall diet quality. Children who consumed whole fruit had better diet quality scores for total fruit, whole fruit, whole grains, dairy, seafood, refined grains, sodium, and empty calories (P ≤ 0.018). Significantly higher HEI-2010 scores for total fruit, whole fruit, fatty acids, sodium, and empty calories, but a lower dairy HEI-2010 score, were identified in children who drank fruit juice (P ≤ 0.038). Vegetable consumption was significantly associated with higher total vegetables, greens/beans, and empty calories, but a lower sodium score (P ≤ 0.027). Children who consumed whole fruit, fruit juice and non-starchy vegetables (P ≤ 0.017), but not white potatoes, had significantly higher total HEI-2010 scores. Reinforcing fruit and 100% fruit juice consumption may indirectly support healthier diets among children. However, underlying associations between fruit and vegetable intakes and overall diet quality should be examined further.