Alpine lake sediments and glacier ice cores retrieved from high mountain regions can provide long-term records of atmospheric deposition of anthropogenic contaminants such as mercury (Hg). In this study, eight lake sediment cores and one glacier ice core were collected from high elevations across the Himalaya-Tibet region to investigate the chronology of atmospheric Hg deposition. Consistent with modeling results, the sediment core records showed higher Hg accumulation rates in the southern slopes of the Himalayas than those in the northern slopes in the recent decades (post-World War II). Despite much lower Hg accumulation rates obtained from the glacier ice core, the temporal trend in the Hg accumulation rates matched very well with that observed from the sediment cores. The combination of the lake sediments and glacier ice core allowed us to reconstruct the longest, high-resolution atmospheric Hg deposition chronology in High Asia. The chronology showed that the Hg deposition rate was low between the 1500s and early 1800, rising at the onset of the Industrial Revolution, followed by a dramatic increase after World War II. The increasing trend continues to the present-day in most of the records, reflecting the continuous increase in anthropogenic Hg emissions from South Asia.