We report on a new type of liquid crystalline cellulosic films with light controllable reversible wettability. The films are prepared from a thermotropic cellulose derivative functionalized with azo-containing groups. These groups exhibit dynamic changes in interfacial properties in response to UV irradiation. The UV irradiation induces trans-to-cis isomerization in the azobenzene moiety, which causes a conformational change in the upper molecular layers of the thin films. These changes originate a hydrophobic to comparatively hydrophilic transformation of the surface. The reversible wettability of the surface results from the cis/trans photo and thermal isomerization. The UV-vis absorption spectra, as well as contact angle measurements with UV irradiation, clearly support the understanding of the phenomenon. This type of surface design enables the amplification of molecular level conformational transitions to macroscopic changes in interface properties using the means of isomerism. This opens new opportunities in surface engineering using eco-friendly cellulose manipulation.