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Methylxanthines were quantified in coffee, tea, and chocolate products. Tarajuilie tea from India, cocoa powder, and cocoa nibs contained the highest levels of methylxanthines. Theobromine, caffeine, and theophylline combined in the ratios observed in tea and chocolate were ingested by coyotes. Although both mixtures induced acute toxicity, the symptoms accompanying the chocolate methylxanthine mimic were preferable. Manipulation of the ratios of methylxanthines in the chocolate mimic led to the identification of a 5:1 theobromine/caffeine mixture as a promising coyote toxicant. This mixture was then administered to coyotes using the coyote lure operative device (CLOD). Mortality occurred in every coyote that ingested any portion of the CLOD contents. These results indicate that mixtures of theobromine and caffeine have the potential to be developed into a selective, effective, and socially acceptable toxicant for the control of pest coyotes.