Synthetic biology enables microbial hosts to produce complex molecules that are

otherwise produced by organisms that are rare or difficult to cultivate, but the structures of these

molecules are limited to chemical reactions catalyzed by natural enzymes. The integration of

artificial metalloenzymes (ArMs) that catalyze abiotic reactions into metabolic networks could

broaden the cache of molecules produced biosynthetically by microorgansms. We report the

assembly of an ArM containing an iridium-porphyrin complex in the cytoplasm of a terpene

producing Escherichia coli by a heterologous heme transport machinery, and insertion of this ArM

into a natural biosynthetic pathway to produce an unnatural terpenoid. This work shows that

synthetic biology and synthetic chemistry, incorporated together in whole cells, can produce

molecules previously inaccessible to nature.

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