Shaped by millions of years of evolution, enzymes have mastered an impressive arsenal of chemical transformations and, in doing so, conquered even the far reaches of chemical space. Enzymes have learned how to effect transformations, which go against the innate reactive preferences of substrates, transformations, which rapidly construct molecular complexity from simple precursors and transformations, which require highly precise control over transition states to obtain the desired product. This catalytic prowess has enabled biosynthetic access to natural products with complex and intriguing architectures as well as valuable biological activities. Understanding and exploiting these compounds and their biological activities has been an active area of research for several decades, with implications in medicinal chemistry and beyond. This, however, requires a viable route for access to said natural products, which continues to serve as a driving factor motivating the chemical total synthesis of complex natural products. However, without enzymes, accessing many natural products is less than straightforward with conventional chemical methods: Cross-coupling reactions typically require prefunctionalization, oxidative manipulations generally demand protecting groups, and asymmetric transformations often necessitate extensive catalyst screening and reaction optimization. Nonsurprisingly, the strategic use of enzymes in natural product synthesis has gained increased popularity in recent years.