The acidity of atmospheric particulate matter regulates its mass, composition, and toxicity and has important consequences for public health, ecosystems and climate. Despite these broad impacts, the global distribution and evolution of aerosol particle acidity are unknown. We used the comprehensive atmospheric multiphase chemistry-climate model EMAC (ECHAM5/MESSy Atmospheric Chemistry) to investigate the main factors that control aerosol particle acidity and uncovered remarkable variability and unexpected trends during the past 50 years in different parts of the world. Aerosol particle acidity decreased strongly over Europe and North America during the past decades while at the same time it increased over Asia. Our simulations revealed that these particle acidity trends are strongly related to changes in the phase partitioning of nitric acid, production of sulfate in aqueous aerosols, and the aerosol hygroscopicity. It is remarkable that the aerosol hygroscopicity (Îº) has increased in many regions following the particle pH. Overall, we find that alkaline compounds, notably ammonium and to a lesser extent crustal cations, regulate the particle pH on a global scale. Given the importance of aerosol particles for the atmospheric energy budget, cloud formation, pollutant deposition, and public health, alkaline species hold the key to control strategies for air quality and climate change.