Land degradation due to mining is a major concern leading to massive losses of biodiversity and ecosystem services. The biomonitoring of metals in mine voids can help to keep track of ecosystem health. The present study was carried out in a large mine void that is presently used for fly ash disposal in the Angul district of Odisha, India. For the biomonitoring of the fly ash, composite soil and plant samples (non-edible as well as edible, naturally growing in and around the mine void) were collected seasonally four times between April 2018 and February 2019 from the sampling locations. We monitored the metal uptake (Al, Cd, Cr, Fe, Mn, Ni, Pb, Zn) and bioaccumulation to assess the bioaccumulation factor (BAF) in the collected plant samples. The Fe concentration was reported to be high in Tragia involucrate (24.82 mg/kg) and Digitaria ciliaris (24.818 mg/kg), while the soil at the study site is also rich in Fe and Al. Higher concentrations of metals in fruit trees such as Psidium guajava and other plants such as Ficus religiosa, Ipomoea batatas, Delonix regia, Digitaria ciliaris, and Cynodon dactylon were reported from nearby areas. Understanding the presence of metals should be a guiding factor for reducing land degradation. Our study stresses the need for corporate commitment to ensure regular biomonitoring and biomonitoring-supported land restoration for degraded mining areas. Sustainable land restoration supported by biomonitoring has the potential to help achieve the global goals of the UN Decade on Restoration: Land Degradation Neutrality (UNCCD) and Sustainable Development Goals (SDGs) 12, 13, and 15.