In　this　work,　self-assembled　gels　were　prepared　with　exfoliated　montmorillonite　and　chitosan　(EMCG)　as　the　adsorbent　for　removing　methyl　orange　(MO)　from　water　in　absence　and　presence　of　methylene　blue　(MB).　Several　techniques　including　scanning　electron　microscope　(SEM),　zeta　potential,　fourier　transform　infrared　spectroscopy　(FTIR)　and　X-ray　photoelectron　spectroscopy　(XPS)　were　used　for　the　characterization　of　the　EMCG　before　and　after　removal　of　MO.　The　EMCG　performed　well　in　the　removal　of　MO　attributing　to　the　electrostatic　attraction,　cation　exchange　and　hydrogen　bond.　The　adsorption　behaviors　were　followed　pseudo-second-order　and　Langmuir　isotherm.　More　surprisingly,　the　maximum　adsorption　capacity　of　MO　was　obviously　enhanced　in　the　presence　of　MB　that　it　increased　from　545　mg　g−1　(absence　of　MB)　to　1060　mg　g−1　with　the　shielding　effect　of　MB　on　EMCG　which　allowed　MO　and　MB　to　alternately　arrange　at　the　adsorption　sites.　This　finding　of　the　synergistic　effect　between　the　two　dyes　on　the　proposed　composite　opens　up　new　vistas　to　imagine　the　enhanced　purification　of　the　wastewater　with　multiple　dyes　co-existed　using　the　multifunctional　adsorbents.　©　2019　Elsevier　Ltd