The objectives of the present study were to characterize good-quality cultivars, identify relationships between local eating preferences and primary compound content, and reveal biofortification potential in tropical root crop species aroids, yams, cassava, and sweet potato. A core sample of about 500 cultivars was assembled to represent the widest agro-morphological diversity. Very high coefficients of variation were found within species for proteins, sugars, cellulose, and mineral contents, whereas starch exhibited the lowest variation. Starch content was negatively correlated with other primary compound contents. For the national dish in Vanuatu, consumers prefer cultivars with high starch content. In contrast, preferences for daily consumption of boiled or roasted tubers are linked to average starch content, indicating great potential for improving primary compounds. Interestingly, relationships between flesh color and requirements for the traditional dish were revealed, suggesting opportunities for biofortification. The data produced will assist breeders in adopting appropriate biofortification strategies.