The efficacy of liquid crystal display (LCD) devices heavily hinges on the alignment of mesogens. In traditional LCDs, mesogens are oriented within substrates using the rubbed polyamide technique, which introduces undesirable contaminants and static charges, compromising device performance. This study presents a novel approach wherein plant-derived cellulose nanocrystals (CNCs) serve as an alternative alignment layer, obviating the need for the conventional rubbed polyamide technique. CNCs, extracted from banana pseudo-stem fibers via acid hydrolysis, are leveraged for alignment layer formation on ITO substrates using a rubbing-free vertical deposition technique. LC devices with various pre-alignment layers, including conventional rubbed polyamide and CNC layers, were fabricated and systematically compared. Through AFM, SEM, and profilometric analyses, we confirmed the presence of micro-sized channels and spindle-like structures of the CNCs, resulting from their self-assembly during vertical deposition. The device with the CNC layer exhibited robust mesogenic alignment and was sensitive to CNC layer thickness. The CNCs' spindle-like structure and self-assembling properties, coupled with vertical deposition, facilitated microchannel formation on the substrate, ensuring homogeneous alignment. The increased surface energy of CNC layers significantly improved mesogenic alignment, as evidenced by polarized optical microscopy and contact angle measurements. Moreover, the influence of these alignment layers extended to dielectric relaxation and transition temperature. Electro-optical properties, including spontaneous polarization, switching time, photoluminescence emission, and P-E hysteresis, were found to be comparable to conventionally rubbed polyimide, all while maintaining transparency. Additionally, CNC layers exhibited ion-capturing capabilities, leading to a reduction in device conductivity. This study underscores the potential of CNCs as an alignment layer for LCD applications, offering advantages such as enhanced wettability, density distributions, and overall orientation.