Biofortified maize, designed as an intervention strategy to prevent vitamin A deficiency, can provide upwards of 15 μg β-carotene per g dry weight. Some varieties also have elevated concentrations of other carotenoids. We conducted a cluster randomized, controlled feeding trial in rural Zambia to test the impact of daily consumption of biofortified maize over a 6-month period on vitamin A status. Serum concentrations of retinol and carotenoids were assessed by high-performance liquid chromatography. Data on circulating carotenoids by intervention group in 679 children are reported here. As previously shown, consumption of this β-carotene-rich maize significantly improved serum β-carotene concentrations (0.273 vs. 0.147 μmol/L, p < 0.001, in this subset of children). Here we show significant increases in α-carotene, β-cryptoxanthin, and zeaxanthin (p < 0.001). There was no impact on lutein or lycopene concentrations. Consumption of biofortified maize can have broader implications beyond the control of vitamin A deficiency (Trial registration: NCT01695148).