Management of metal(loid) tailings at historic sites presents environmental hazards usually requiring rehabilitation to mitigate pollution risks. Strategies employed include capping or establishing vegetation directly, which requires tailings assessments to determine suitable rehabilitation approaches. Assessments are typically geochemical analyses, but plant based approaches may provide a more accurate measure of revegetation success although they are often limited to germination indices. This study uses the plant bioassay (Rhizotest¿) with common geochemical assessment to predict plant uptake of metal(loid)s and the subsequent likely rehabilitation success. Pb/Zn tailings from five legacy sites within the UK and Ireland were characterized for pH, EC, water soluble and CaCl2-extractable content and aqua regia extractable content. Uptake of Sb, As, Cd, Cu, Ca, Mg, Mn, Zn, Pb was determined in shoots and roots of Lolium perenne. Total Zn, Pb, Sb, Cd and As in tailings ranged from 694 to 2683 mg kg¿1, 1252 to 8072 mg kg¿1, 14 to 148 mg kg¿1, 1.3 to 44 mg kg¿1 and 1.3 to 45 mg kg¿1, respectively. The only correlation found between total and water soluble or CaCl2-extractable metal(loid) contents was for Cd, where r = 0.8 for total and CaCl2-extractable fractions. Limited uptake and translocation risk was identified for major contaminants Zn and Pb in most tailings samples but in some cases exceedance of phytotoxic threshold values occurred that was not reflected in geochemical analysis. Crucially, although total Cd and Sb content was relatively low (< 20 mg kg¿1) in some tailings, elevated plant content for some samples highlights phytotoxic risk from minor elements. Results indicate that screening based on geochemical content is not sufficiently predictive of metal(loid) phytoavailability to reliably inform mine rehabilitation strategies. We therefore strongly recommend that geochemical analyses are supplemented with plant based bioassay to plan mine tailings revegetation and reduce risk of wider ecosystem metal(loid) transfer.