Abstract Often the first point of contact between predator and prey, mammalian canine teeth are essential for killing, dismembering and consuming prey. Yet despite their importance, few associations among shape, function and phylogeny are established. We undertook the first comprehensive analysis of canine tooth shape across predatory mammals (Carnivora, Didelphimorphia and Dasyuromorphia), integrating shape analysis with function of this fundamental feature. Shape was quantified using three-dimensional geometric morphometrics and cross-sectional sharpness. Canines vary in three main ways (sharpness, robustness and curvature) which vary with diet, killing behaviour and phylogeny. Slender, sharp canines are associated with carnivores such as felids that target the neck of their prey and primarily consume the ‘softer’ parts of a carcass. Robust, blunt canines are found in mustelids and dasyurids that typically consume ‘harder’ materials, such as bone, or bite into skulls. Differences in the killing behaviours of felids and canids probably result in more curved canines in the latter, which act as hooks to hold prey. We find functional specialization in the upper and lower canines of individuals and across the major mammalian clades. These patterns demonstrate how canine teeth are adapted to suit diverse diets and hunting styles, enabling mammals to become some of nature's most successful predators.