The aim of this research was simple preparation of grafted 1,3,5-Tris (2-hydroxyethyl isocyanurate) to the chitosan surface by using EDTA linker (CS-EDTA-THEIC) through a green and inexpensive procedure. The obtained nanomaterial was characterized via different spectroscopic, microscopic and analytical methods. Various techniques and methods namely Fourier transform infrared (FTIR), field emission scanning electron microscopy (FESEM), simultaneous thermogravimetric analysis (STA), X-ray diffraction analysis (XRD) were utilized to identify the nanomaterial. This bio-based CS-EDTA-THEIC network contains appropriate basic and acidic active sites to act as a multifunctional catalyst. Finally, the CS-EDTA-THEIC nanomaterial was used in the multicomponent reaction for synthesis of 4H-pyrans and 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 five times without significant loss of its activity.