Structural analysis of natural products remains challenging due to their inherent complexity and limited availability. By solving nine chemically diverse natural products of high priority that have resisted reported 3D structures for years, we demonstrate that microcrystal electron diffraction (MicroED) can systematically and feasibly be applied to natural-product structure elucidation on samples that were previously unattainable by other structural methods. In addition, using microgram quantities of material and side-stepping the process to create large single crystals, the success rate is still comparable to other techniques on a general sample using larger amounts of the sample. We suggest that MicroED is not only a necessary technique but also a general and efficient tool for many applications.