The study investigates the effect of the organic compound representing the cellulose derivative - sodium salt of carboxymethyl cellulose (CMC/Na) on the structure of the main component of bentonite (B) - montmorillonite (MMT). Structural analysis revealed that the CMC/Na of different viscosity interacts with the mineral only via surface adsorption, causing at the same time partial or full delamination of its layered structure. This was confirmed by the XRD diffraction tests. Such polymer destructive influence on the structure of the modified main component of the bentonite limits the use of its composites as an independent binder in moulding sand technology, but does not exclude it from acting as an additive being a lustrous carbon carrier. According to the IR spectra of the B/CMC/Na materials, it can be stated that the interaction between the organic and inorganic parts is based on the formation of hydrogen bonds. That kind of the interpretation applies especially to the MMT modified in the bentonite with a lower viscosity polymer. The characteristics of the main IR absorption bands for composites with a higher viscosity polymer indicates the formation of less stable structures suggesting the random nature of the hydrogen bonds formation.