The use of bioenergy plants for the cleaning of polluted lands (phytoremediation) is an innovative strategy to derive additional benefits (i.e. phytoproducts) from such remediation activities. There are multitude of plant species that can be used for concurrent phytoremedaiton as well as obtaining useful end products such as bioethanol, biodiesel, fiber, wood, charcoal, alkaloids, bioplastics etc. during the clean-up process. Among the phytoproducts, bioenergy is getting worldwide attention as it considered as a clean and a versatile source of energy. However, there are many outstanding questions to be answered before the large-scale production of bioenergy from polluted lands. In this letter, we briefly report the sustainability challenges for coupling phytoremediation with bioenergy production from polluted lands.