The aim of this study is to synthesis of pyrrole derivatives based on phenacyl bromide and amine, which is promoted by a green and heterogeneous chitosan-based catalyst under optimal laboratory conditions through the multi-component reaction strategy namely Hantzsch pyrrole synthesis. This bio-based CS-EDTA-THEIC network contains appropriate basic and acidic active sites to act as a multifunctional catalyst. Indeed, the CS-EDTA-THEIC nanomaterial used in the multicomponent reaction for synthesis of pyrrole derivatives showed excellent yields in short reaction times. Furthermore, the CS-EDTA-THEIC network, as a heterogeneous catalyst, illustrated magnificent reusability and can be used at least six times without significant loss of its activity.