The current research focuses on the development of novel mycotoxins adsorbents using zwitterionic surfactants modified montmorillonites (ZMts) for simultaneous removal of highly health-hazardous polar aflatoxin B-1 (AFB(1)) and low polar zearalenone (ZER). Two types of ZMts including dodecyl dimethyl betaine (BS-12) and lauramidopropyl betaine (LAB-35) modified montmorillonites (BS-12/Mts and LAB-35/Mts) were fabricated, and the structural, interfacial and textural features of which were explored by different techniques. It is indicated that ZMts have different structural configurations based on the surfactant type and loadings, convert from hydrophilic to hydrophobic property, with a mesoporous network inherited from Mt. The resultant adsorbents show significant improvements on the detoxification efficiency of both AFB(1) and ZER. pH has little effect on the adsorption of ZMts, suggesting no desorption happens, The adsorption mechanisms of raw Mt, BS-12/Mts and LAB-35/Mts to AFB(1) and ZER were proposed based on the characterizations and adsorption isotherms. This study demonstrates that ZMts possess simultaneous detoxification functions to mycotoxins with different polarities, and provides new insights into development of versatile mycotoxins adsorbents.