(1) Background: Breastmilk provides all the nutrition an infant requires between 0–6 months. After that, complementary foods are needed to meet the child’s increasing energy and nutrient requirements. Inadequate energy and nutrient intake may lead to growth faltering, impaired neurodevelopment, and increased disease risk. While the importance of early life nutrition is well recognized, there are few investigations assessing the nutritional adequacy of Australian children <24 months. Here, we describe usual energy and nutrient intake distributions, including the prevalence of inadequate intakes and exceeding the upper limit (UL), in a national sample of Australian children 6– 24 months and infants < six months who had commenced solids and/or formula. (2) Methods: Dietary intakes were assessed using a one-day food record for 976 children with a repeat one-day record in a random subset. (3) Results: Based on the Nutrient Reference Values for Australia and New Zealand, children’s intakes were above the Adequate Intake or Estimated Average Requirement for most nutrients. Exceptions were iron and zinc where the prevalence of inadequacy was estimated to be 90% and 20%, respectively, for infants aged 6–11.9 months. Low iron intake was also observed in one quarter of toddlers 12–24 months. On average, children consumed 10% more energy than predicted based on Estimated Energy Requirements, and ~10% were classified as overweight based on their weight for length. One third of toddlers exceeded the tolerable upper limit for sodium and consumed > 1000 mg/day. Of the children under six months, 18% and 43% exceeded the UL for vitamin A (retinol) and zinc. (4) Conclusions: Compared to nutrient reference values, diets were sufficient for most nutrients; however, iron was a limiting nutrient for infants aged 6–11.9 months and toddlers 12–24 months potentially putting them at risk for iron deficiency. Excessive sodium intake among toddlers is a concern as this may increase the risk for hypertension.