Per-and polyfluoroalkyl substances (PFASs) have gained importance since the 1950s and are integral components of most industrial and consumer products. The objective of this study is to critically review the distributions of two PFAS compounds, perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS), in groundwaters worldwide, analyze their sources and identify current challenges. We also assess the data availability of PFOA and PFOS, and gaps in terms of geographical coverage, which is critical for global water resources management. PFOA in groundwater varied from below the level of quantification to 6570 μg L-1, and PFOS varied from below the level of quantification to 68,900 μg L−1. A clear disparity is observed, with studies being concentrated in certain developed regions, whereas other regions experience a deficit due to a lack of awareness and access to advanced facilities. Developed countries in Europe and the United States show that contamination from PFOA and PFOS is from primary sources of PFAS substances, and nonindustrial sources are the major contributors in Asia. Given the contribution of groundwater to the drinking water supply, the legislation and guidelines on PFAS need to be regularly examined and updated. The need for systematic assessment of groundwater for PFAS contamination encompassing the least studied regions is emphasized. More focus is required on the transport of these substances from groundwater to humans, either through the drinking water cycle or through bioaccumulation in organic consumables, and on studying their impact on human health.