The samples of organic-modified clays based on a Wyoming SWy-2 sodium montmorillonite (Na+-Mt) with the cationic surfactant hydroxyethylalkyl imidazoline (HEAI) and the amphoteric surfactant oley-lamidopropyl betaine (OAPB) were synthesized via a cation exchange process. The obtained materials were characterized using XRD analysis, ATR-FTIR spectroscopy, SEM, BET and Water contact angle measurements. The potential sites of binding of OAPB and HEAI to the mineral surface were determined by the DFT calculations. For the variants of the structure of the complex, DFT calculations is performed and the interaction energy of the surfactant and clay mineral is estimated. (C) 2017 Elsevier B.V. All rights reserved.