Excess potentially toxic metals (PTMs) in soils require ad hoc approaches to salvage. Hence, this study explored the shoot accumulation of cadmium (Cd), lead (Pb), and zinc (Zn) by herbaceous plants growing under previously established Salix and Populus clones Short Rotation Coppice (SRC) with compost and sewage sludge applications in an abandoned metallurgical site, Podlesí, Czech Republic; PTM decontamination of soils. Soils within the SRC experimental site and outside considered as control were analyzed for their chemical properties by multi-analytical techniques. Shoots of spontaneously growing herbaceous plants under trees in the site and without trees in control were determined for pseudo-total Cd, Pb, and Zn contents. Moderately to slightly acid soils, high cation exchange capacity, and C/N ratio supported mineralization and relative mobility of total Cd (7.7–9.76), Pb (1541–1929), and Zn (245–320 mg kg−1) in soils. Although soil amendments improved chemical properties, compost application supported higher species richness than sewage sludge. Over 95% of plants accumulated Cd and Zn above the WHO threshold and green fodder in the Czech Republic, with 36% Pb above the regional limit (40 mg kg−1). Approximately 100, 50, and 6% of herbaceous species had Cd, Pb, and Zn accumulation, respectively, higher than published average upper limits in plants (0.2 Cd, 10 Pb, and 150 Zn mg kg−1). Dicots recorded higher Cd content, Tenacetum vulgare (L.), Hypericum maculatum (Crantz), and Cirsium arvense (L.); Stachys palustris (L.), Lamium perpereum (L.), and Campanula patula (L.) for Pb; Glechoma hederaceae (L.), C. patula, and C. arvense for Zn in all treatments. Appropriate soil amelioration of SRC-supported PTM mobility and excess herbaceous species shoot accumulation, growth, and richness.