In the present work, MgFe2O4–bentonite nanocomposite was studied for the photodegradation of malathion and p-nitrophenol as model pollutants. The interactions between MgFe2O4 and bentonite were studied employing XPS, Mӧssbauer, and band gap potential studies. The red shifting in the XPS peaks and FT-IR bands of nanocomposite pinpointed the existence of strong interactions between MgFe2O4 and bentonite. Mössbauer studies revealed increased absorption area corresponding to the doublet assigned to the superparamagnetic fraction of MgFe2O4 NPs in nanocomposite. It signified hindrance in the growth of MgFe2O4 in the presence of bentonite. The nanocomposite showed admirable photodegradation efficiency of 90% for malathion and 86% for p-nitrophenol which was higher than pristine MgFe2O4. The degradation mechanism of malathion and p-nitrophenol was predicted using scavenging studies and GC–MS analysis. The nanocomposite also displayed synergistic removal of metal ions and photodegradation of organic contaminants. It is a potential candidate for remediation of inorganic and organic contaminants.Graphical abstract: