Asbestos exposure has been linked to adverse human health effects including asbestosis and mesothelioma. As such, mining and utilization of asbestos is restricted or has been banned in about 50 countries since 1990. Nevertheless, abandoned asbestos mines, mostly in serpentine areas, persist as sources of hazardous airborne fibers. Revegetation of asbestos mine spoils has been proposed as a way by which to stabilize asbestos-bearing substrate, thereby reducing fiber dispersion into the air. No study to date, however, has evaluated the revegetation's effectiveness of reducing airborne asbestos pollution. In this study, we evaluated the effect of natural revegetation on the air dispersion of asbestos fibers from asbestos-rich serpentine lithosoils at an abandoned chrysotile mine. Air sampling of vegetated and barren plots within the mine demonstrated that vegetative cover significantly reduced asbestos dispersion into the air (50% reduction with 15–40% vegetative cover). Additionally, the effectiveness of several native, locally collected serpentine-tolerant species to revegetate the asbestos mine spoil, including Minuartia and Thymus species, was evaluated. Mat-forming, serpentine endemic Thymus sp. proved to be particularly effective at revegetating the mine spoil, having high transplantation survival, growth rates, and reproductive output.