Abstract17O NMR spectroscopy has been the subject of vivid interest in recent years, because there is increasing evidence that it can provide unique insight into the structure and reactivity of many molecules and materials. However, due to the very poor natural abundance of oxygen‐17, 17O labeling is generally a prerequisite. This is a real obstacle for most research groups, because of the high costs and/or strong experimental constraints of the most frequently used 17O‐labeling schemes. Here, we show for the first time that mechanosynthesis offers unique opportunities for enriching in 17O a variety of organic and inorganic precursors of synthetic interest. The protocols are fast, user‐friendly, and low‐cost, which makes them highly attractive for a broad research community, and their suitability for 17O solid‐state NMR applications is demonstrated.