The synergistic relationship between arbuscular mycorrhizal fungi and plant species may play a key role in phytoremediation of arsenic(As)-contaminated soils. By using modified Leonard jars, we investigated both the distinct and integrative roles of arbuscular mycorrhizal fungi (AMF–Acaulospora scrobiculata) and rhizobia (BH-ICB-A8) isolated from As-contaminated soil on the capacity of Anadenanthera peregrina to reclaim arsenate [As(V)] from soil. AMF inoculation greatly increased plant phosphorous nutrition, as reflected in greater growth, and increased As-concentrations in the roots and shoots. While rhizobia inoculation alone increased nitrogen nutrition it did not promote plant growth or As-uptake. Rhizobia and AMF inoculation together had synergistic effects, however, increasing both the growth and the As-phytoremediation capacity of A. peregrina. Joint inoculation with rhizobia and AMF should therefore be considered a potential technique for rehabilitating As-contaminated areas using A. peregrina.