To understand the role of vegetation and soil in regulating atmospheric Hg⁰, exchange fluxes and isotope signatures of Hg were characterized using a dynamic flux bag/chamber at the atmosphere–foliage/soil interfaces at the Davos-Seehornwald forest, Switzerland. The foliage was a net Hg⁰ sink and took up preferentially the light Hg isotopes, consequently resulting in large shifts (-3.27‰) in δ²⁰²Hg values. The soil served mostly as net sources of atmospheric Hg⁰ with higher Hg⁰ emission from the moss-covered soils than from bare soils. The negative shift of δ²⁰²Hg and Δ¹⁹⁹Hg values of the efflux air relative to ambient air and the Δ¹⁹⁹Hg/Δ²⁰¹Hg ratio among ambient air, efflux air, and soil pore gas highlight that Hg⁰ re-emission was strongly constrained by soil pore gas evasion together with microbial reduction. The isotopic mass balance model indicates 8.4 times higher Hg⁰ emission caused by pore gas evasion than surface soil photoreduction. Deposition of atmospheric Hg⁰ to soil was noticeably 3.2 times higher than that to foliage, reflecting the high significance of the soil to influence atmospheric Hg⁰ isotope signatures. This study improves our understanding of Hg atmosphere–foliage/soil exchange in subalpine coniferous forests, which is indispensable in the model assessment of forest Hg biogeochemical cycling.