Abstract: In this study, we developed montmorillonite modification using Gum arabic hydrothermal carbon (MMT@GC), which was further surface modified by dual-ligand cerium metal organic framework (Ce-MOF) to obtain MMT@GC@PA-MOF (the second ligand is phytic acid) and MMT@GC@TA-MOF (the second ligand is tannic acid) fillers and incorporated them into epoxy resin (EP). It is found that two types of dual-ligand Ce-MOF can enhance the barrier-active anti-corrosion, mechanical properties, fluorescence detection, and flame resistance of MMT@GC sheet for EP composite. For EP-MMT@GC@PA-MOF, the low frequency impedance can be maintained after 40 d immersion. Also, the EP-MMT@GC@PA-MOF shows good flame-retardant properties relying on its good carbon forming capability, which increased 17.2% than bare EP according to the thermogravimetric test. In comparison, the MMT@GC@TA-MOF shows suitable acid and iron ions stimulus-release characteristics, which endow EP with good active anti-corrosion effect and corrosion detection property to accurately reports the immersion zone and mechanical damage zone only after 2 d immersion in 3.5wt% NaCl. More importantly, compared to bare EP, at least a 73.4% increase in adhesion force and a 27.5% increase in tensile strength of EP-MMT@GC@PA-MOF and EP-MMT@GC@TA-MOF can ensure the long-term service of the multifunctional composites. This work demonstrates a versatile strategy for designing tailorable, multi-responsive epoxy composites via the in-situ growth of dual-ligand Ce-MOF (using TA or PA) on bio-derived GC-modified 2D templates.