Metalloid is an element with chemical properties intermediate between metals and semiconductors. Metalloids such as heavy metals are toxic to most organisms when present in excessive concentrations in agricultural soils. Several research studies indicate that microorganisms in soil are more sensitive to heavy metal stress than the other soil flora and fauna on the same soil. Contamination of soils with metals is one of the rapidly growing and most concerning environmental hazards in this century. Reports indicate that certain plants and microorganisms such as fungi, when they interact in the soil play a significant role in phytoremediation. Phytoremediation is a sustainable, cost-effective, and environment-friendly ecological approach for reclamation of metal-contaminated soils. This chapter discusses the diverse use of plants and fungi in the remediation and removal of metalloids from contaminated soil. Fungi are one of the most potent bioresources for remediation, as several reports indicate that the fungi are more tolerant of heavy metals than other microorganisms.