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Objectives: We evaluate the potential of paired isotopic analysis of bone carbonate and collagen to examine the diet of post‐medieval human and animal populations from England (17th–19th c.), including, for the first time, manufacturing towns in northern England. The potential for identifying C4 crop consumption is explored alongside regional and local patterning in diet by sex and socioeconomic status. Materials and Methods: Humans (n = 216) and animals (n = 168) were analyzed from sites in London and northern England for both carbon and nitrogen isotopes of bone collagen (훿13Ccoll, 훿15Ncoll). Isotopic analysis of bone carbonates (훿13Ccarb, 훿18Ocarb) was carried out on all humans and 27 animals, using Fourier transform infrared spectroscopy–attenuated total reflectance to assess diagenesis. Results: Variations in diet were observed between and within different populations by geographical location and socioeconomic status. Three pigs and one cow consumed C4 resources, indicating the availability of C4‐fed animal protein. Londoners consumed more animal and marine protein and C4 resources. Middle‐ and upper‐class populations from both London and northern populations also had greater access to these foods compared to those of lower status in the same regions. Discussion: This substantial multi‐isotope dataset deriving from bone carbonate and collagen combined from diverse post‐medieval urban communities enabled, for the first time, the biomolecular identification of the dynamics of C4 consumption (cane sugar/maize) in England, providing insight into the dynamics of food globalization during this period. We also add substantially to the animal dataset for post‐medieval England, providing further insight into animal management during a key moment of agricultural change. [ABSTRACT FROM AUTHOR]