Accumulating isotopic evidence from fossil hominin tooth enamel has provided unexpected insights into early hominin dietary ecology. Among the South African australopiths, these data demonstrate significant contributions to the diet of carbon originally fixed by C
4
photosynthesis, consisting of C
4
tropical/savannah grasses and certain sedges, and/or animals eating C
4
foods. Moreover, high-resolution analysis of tooth enamel reveals strong intra-tooth variability in many cases, suggesting seasonal-scale dietary shifts. This pattern is quite unlike that seen in any great apes, even ‘savannah’ chimpanzees. The overall proportions of C
4
input persisted for well over a million years, even while environments shifted from relatively closed (
ca
3 Ma) to open conditions after
ca
1.8 Ma. Data from East Africa suggest a more extreme scenario, where results for
Paranthropus boisei
indicate a diet dominated (approx. 80%) by C
4
plants, in spite of indications from their powerful ‘nutcracker’ morphology for diets of hard objects. We argue that such evidence for engagement with C
4
food resources may mark a fundamental transition in the evolution of hominin lineages, and that the pattern had antecedents prior to the emergence of
Australopithecus africanus
. Since new isotopic evidence from Aramis suggests that it was not present in
Ardipithecus ramidus
at 4.4 Ma, we suggest that the origins lie in the period between 3 and 4 Myr ago.