Excavations at Abu Hureyra, Syria, during the 1970s exposed a long sequence of occupation spanning the transition from hunting-and-gathering to agriculture. Dung spherulites preserved within curated flotation samples from Epipalaeolithic (ca. 13,300-11,400 calBP) and Neolithic (ca. 10,600-7,800 calBP) occupations are examined here alongside archaeological, archaeobotanical, and zooarchaeological data to consider animal management, fuel selection, and various uses of dung. Spherulites were present throughout the entire sequence in varying concentrations. Using a new method to quantify spherulites, exclusion criteria were developed to eliminate samples possibly contaminated with modern dung, strengthening observations of ancient human behavior. Darkened spherulites within an Epipalaeolithic 1B firepit (12,800-12,300 calBP) indicate burning between 500-700°C, documenting early use of dung fuel by hunter-gatherers as a supplement to wood, coeval with a dramatic shift to rectilinear architecture, increasing proportions of wild sheep and aurochsen, reduced emphasis on small game, and elevated dung concentrations immediately outside the 1B dwelling. Combined, these observations suggest that small numbers of live animals (possibly wild sheep) were tended on-site by Epipalaeolithic hunter-gatherers to supplement gazelle hunting, raising the question of whether early experiments in animal management emerged contemporaneously with, or pre-date, cultivation. Dung was used to prepare plaster floors during the Neolithic and continued to be burned as a supplemental fuel, indicating that spherulites were deposited via multiple human- and animal-related pathways. This has important implications for interpretations of archaeobotanical assemblages across the region. Spherulite concentrations dropped abruptly during Neolithic 2B (9,300-8,000 calBP) and 2C (8,000-7,800 calBP), when sheep/goat herding surpassed gazelle hunting, possibly corresponding with movement of animals away from the site as herd sizes increased. As hunter-gatherers at Abu Hureyra began interacting with wild taxa in different ways, they set in motion a remarkable transformation in the ways people interacted with animals, plants, and their environment.