In this study, we observed the Geyser phenomenon that occurs in a small-diameter two-phase closed thermosyphon (confinement number of 0.245). This phenomenon interferes with the natural circulation of the internal working fluid and increases the thermal resistance of the system. This study attempts to improve the thermal performance of the system using cellulose nanofiber as the working fluid and hydrophilic surface modification at the inner surface of the evaporator section. As a result, the total thermal resistance showed average reduction rates of 47.51%, 36.69%, and 22.56% at filling ratios of 0.25, 0.5, and 0.75, respectively.