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Zinc distribution and speciation within different organs (root, petiole, and leaf) of the edible plant Eruca vesicaria L. Cavalieri were determined using synchrotron microbeam X-ray techniques (XRF microtomography and mu-XANES) for plants grown in polluted soil with or without compost amendment. Data on soil derived from different extraction procedures and using mu-XANES analyses on rhizospheric soil indicated that compost amendment did not significantly influence the Zn speciation and availability in soil. However, major differences were observed within the plants. Plants grown in the presence of compost were able to partly block zinc immediately outside the root endodermis in the form of zinc-phytate, while a smaller Zn fraction was allowed to xylem transport as zinc-citrate. In the leaves, zinc was largely excluded from leaf cells, and about approximately 50% was in the form of phosphate precipitates, and the other 50% was complexed by cysteine and histidine residues. The reported data provide new information concerning the mechanisms of zinc tolerance in E. vesicaria L. Cavalieri, a very common edible plant in Mediterranean regions, and on the role of compost in influencing the molecular strategies involved in zinc uptake and detoxification.