The use of waste materials as organic amendments in soil remediation can affect metal solubility; this interaction will vary with the characteristics of the organic matter that is added to the soil. A pot experiment was carried out in a calcareous, metal-polluted soil, using Beta maritima L. as an indicator species for the treatment effects on metal solubility. The treatments were: fresh solid olive husk, a mature compost, their respective water extracts (as the most reactive and biodegradable fraction) and an unamended, control soil. The compost reduced metal availability and plant uptake, while fresh olive husk favoured Mn bioavailability and produced phytotoxicity. The water-soluble extract from fresh solid olive husk also provoked elevated Mn solubility in soil, but did not increase Mn uptake by plants. The application of water-soluble organic matter obtained from compost did not affect heavy metal solubility significantly. Therefore, composted olive husk seems to be the most-appropriate material for the development of bioremediation strategies.