The bioaccessibility and bioavailability of iron from 12 Andean potato clones were estimated using an in vitro gastrointestinal digestion procedure and the Caco-2 cell line as a model of human intestine, with ferritin formation as a marker of iron absorption. We first showed that 63.7% (for the genotype CIP-311422.016) to 79.0% (for the genotype CIP-311575.003) of the iron is released from the potato tuber matrix during in vitro gastrointestinal digestion and is therefore available at the intestinal level. On average, 32 and 24.5% of the hydrophilic bioactive components, vitamin C and chlorogenic acid, respectively, were also bioaccessible from boiled tubers. Intestinal absorption of intrinsic iron from potato tubers could not be detected using our in vitro Caco-2 cell model. When an extrinsic source of iron (20 μM FeCl3 and 1 mM ascorbic acid) was added to the digestion mixture, iron absorption varied from 1.8 to 8% for the genotypes CIP-311422.016 and CIP-311624.021, respectively, as compared to the reference control. Principal component analysis revealed negative relationships between bioavailable iron values and phenolic concentrations, whereas vitamin C concentrations were positively associated with the ferritin values. Further controlled intervention trials would be needed to conclusively assess the bioavailability of intrinsic iron from potato tubers.