The forest ecosystem is a significant pool for capturing atmospheric mercury (Hg) deposition, with most Hg accumulating in forest soils. As secondary forests now dominate global forest cover, they are particularly sensitive to changes in ambient temperature. However, the impact of these changes on Hg dynamics in secondary forests remains poorly understood. Here, we quantified Hg inputs, outputs, and mass balances in two secondary forests in China, each with different ambient temperatures. We found that elevated ambient temperature (~1.0℃) advanced the germination of leaves by 2-3 days and extended the growing season by approximately one week, resulting in increased litterfall biomass by 1.18 Mg hm-2 yr-1 and a thicker litterfall layer by 0.22cm over 34 years. This temperature rise also facilitated Hg methylation within forest and enhanced methylmercury (MeHg) export, heightening the potential risk of MeHg exposure to surrounding ecosystems. Additionally, higher ambient temperature not only increased soil Hg emissions (2.75µgm-2 yr-1) but also led to significant Hg deposition via litterfall (9.26µgm-2 yr-1), resulting in a net annual Hg deposition of 6.88µgm-2 yr-1. This net Hg deposition accumulated in the topsoil, increasing the Hg pool by 0.51mgm-2 in organic and 0-10cm mineral soil horizons. Our findings suggest that even a ~1.0℃ temperature rise could enhance the role of secondary forests as atmospheric Hg sink by 45.10%. Therefore, the impact of ongoing climate warming on Hg cycling and pools in forests should receive increased attention and warrants further research.