Increasing atmospheric CO2 drives ocean acidification, with some of the fastest rates observed on Arctic shelves. Lowest pH levels occur near the coasts due to the additional effects of land-derived carbon sources. However, the impact of anthropogenic climate change on seawater acidity mediated by increasing permafrost thaw and coastal erosion remains unknown. Here, we find that the increase in organic matter release by coastal permafrost erosion over the 20th century enhances the interannual variability of seawater pH in Arctic near-shore areas. As a consequence, carbonate undersaturation events, stressing marine ecosystems, become more frequent, intense, and longer-lasting. We account for synergistic effects of anthropogenic climate change by combining increasing atmospheric CO2 levels and coastal erosion rates, utilizing a novel global model with high-resolution grid refinement towards coastal regions and improved process representation of shelf-specific carbon dynamics. By considering the role of coastal permafrost erosion, we conclude that critical Arctic Ocean acidification states will emerge earlier than simulated by the current generation of Earth system models. Our results emphasize the importance of understanding permafrost-ocean interactions and their increasing impact on marine ecosystems, especially in the rapidly changing Arctic region.