The self-assembly is the primary mechanism responsible for organization of the components into ordered and/or functional structures found in nature. The liquid crystals (LCs) and cellulose nanocrystals (CNCs) display strong intermolecular interactions, forming different ordered structures. Using this property, a new nanocomposite based on LC/CNC mixtures have been designed and prepared as molecular films. The Langmuir technique was used to prepare the investigated materials and study their properties. We have used three different LCs - 5CB, 5FCB, and 5PCH, combined with CNC at the air-water interphase. The study aimed to check if obtained nanocomposites benefit from the advantages of both constituents and results in new quality. Such natural derived systems could be used to manufacture materials with specific properties for task-specific applications. This paper focuses on the characterization of the surface and its features (morphology, topography, roughness) and reconstruction of the obtained surfaces in the 3D image. Studied systems have shown different surface characteristics related to the intermolecular interactions between the liquid crystal and cellulose nanocrystals. The computational methods implemented in Gwyddion software has been used to characterize the obtained surfaces. The Brewster Angle Microscopy (BAM) has been used for imaging of the molecular ordering in the composed LC/CNC Langmuir film. (C) 2020 Elsevier B.V. All rights reserved.