Individual specialization, which describes whether populations are comprised of dietary generalists or specialists, has profound ecological and evolutionary implications. However, few studies have quantified individual specialization within and between sympatric species that are functionally similar but have different foraging modes. We assessed the relationship between individual specialization, isotopic niche metrics and foraging behaviour of two marine predators with contrasting foraging modes: pelagic foraging female South American fur seals (Arctocephalus australis) and benthic foraging female southern sea lions (Otaria byronia). Stable isotope analysis of carbon and nitrogen was conducted along the length of adult female vibrissae to determine isotopic niche metrics and the degree of individual specialization. Vibrissae integrated time ranged between 1.1 and 5.5 years, depending on vibrissae length. We found limited overlap in dietary niche-space. Broader population niche sizes were associated with higher degrees of individual specialization, while narrower population niches with lower degrees of individual specialization. The degree of individual specialization was influenced by pelagic and benthic foraging modes. Specifically, South American fur seals, foraging in dynamic pelagic environments with abundant but similar prey, comprised specialist populations composed of generalist individuals. In contrast, benthic southern sea lions foraging in habitats with diverse but less abundant prey had more generalist populations composed of highly specialized individuals. We hypothesize that differences in specialization within and between populations were related to prey availability and habitat differences. Our study supports growing body of literature highlighting that individual specialization is a critical factor in shaping the ecological niche of higher marine predators.