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Drop-in biohydrocarbons have the potential to directly replace fossil-based products due to their chemical and physical similarity, and are fully compatible with the existing petroleum processing, distribution, and components infrastructure. Herein, we will show the structure and function of a cytochrome P450, a terminal (poly-unsaturated) olefin-producing decarboxylase, which enables the use of unsaturated fatty acids as feedstocks for alkene production. The enzyme exploits a distinct molecular mechanism for substrate binding and chemoselectivity comparing to the CYP-decarboxylases characterized thus far. The broad spectrum of substrates metabolized, and less-restrictive reaction conditions represent an advance toward the development of biological routes for the production of sustainable hydrocarbons, which is an urgent need for the mitigation of climate change and reduction of the dependence on …