Iron transport into the CNS is still not completely understood. Using a brain perfusion technique in rats, we have shown a significant brain capillary uptake of circulating transferrin (Tf)‐bound and free ⁵⁹Fe (1 nm) at rates of 136 ± 26 and 182 ± 23 μL/g/min, respectively, while their respective transport rates into brain parenchyma were 1.68 ± 0.56 and 1.52 ± 0.48 μL/g/min. Regional Tf receptor density (B_max) in brain endothelium determined with ¹²⁵I‐holo‐Tf correlated well with ⁵⁹Fe‐Tf regional brain uptake rates reflecting significant vascular association of iron. Tf‐bound and free circulating ⁵⁹Fe were sequestered by the choroid plexus and transported into the CSF at low rates of 0.17 ± 0.01 and 0.09 ± 0.02 μL/min/g, respectively, consistent with a 10‐fold brain‐CSF concentration gradient for ⁵⁹Fe, Tf‐bound or free. We conclude that transport of circulating Tf‐bound and free iron could be equally important for its delivery to the CNS. Moreover, data suggest that entry of Tf‐bound and free iron into the CNS is determined by (i) its initial sequestration by brain capillaries and choroid plexus, and (ii) subsequent controlled and slow release from vascular structures into brain interstitial fluid and CSF.