A method that enabled the formulation of lubricating oleogels using dried cellulose nanofibers (CNFs) as an eco-friendly thickener in castor oil was studied. In their dehydrated state, strong hydrogen bonding between nanofibers and high hydrophilicity are the main obstacles to their dispersion in oil. Hence, clusters of dried CNFs had to be previously detached by their dispersion in water. The resulting hydrogels were then subjected to methanol washes to displace the water from the nanofibers. After centrifugation, the methanol-wetted precipitate was readily dispersed in castor oil, forming an oleogel once the methanol was removed. Optimization was conducted in terms of the following variables: (a) hydrogel processing method; (b) hydrogel pH; (c) methanol/hydrogel ratio; (d) number of washes; and (e) oleogel CNF concentration. Their effect on the oleogel linear viscoelastic behavior was analyzed. In general, they demonstrated a prevailing elastic behavior denoted by a well-developed plateau region. The CNF concentration was found to have a more remarkable impact on the oleogels’ rheological behavior than any other variable studied. Hence, substantial differences were observed between 1 and 2 wt.%. The CNFs exhibited a very remarkable thickening capacity in castor oil, achieving a plateau modulus of ca. 700 Pa with just 2 wt.%. Moreover, the resulting oleogels maintained a uniform texture even after one year of storage. This indicates that the oleogels were both homogeneous and storage stable, effectively overcoming the stability issues associated with direct dispersion of dried CNFs in castor oil.

(1) Background: Developing fully bio-based lubricating greases requires eco-friendly alternatives to conventional harmful components. This study highlights unmodified nanocellulose as an effective structuring agent in vegetable oils, enabling 100% bio-based formulations. (2) Methods: Three bio-based greases were formulated using 1.4 wt.% cellulose nanofibers (CNFs), derived from elm wood pulp through mechanical and chemical pretreatment, as thickening agents in castor oil. Their tribological performance was evaluated under varying temperatures and contact loads and compared to a reference lithium-based grease (LBG) containing 14 wt.% thickener, also formulated with castor oil. (3) Results: Among the CNFs, the unbleached variant (CNF-U) which retained the highest lignin content exhibited the highest coefficient of friction (COF), ranging from 0.09 to 0.14 across test conditions, along with a wear scar diameter of approximately 615 µm at 60 °C. Notable differences in shear stress sensitivity were observed between mechanically and chemically treated nanofibers. The TEMPO-oxidized nanofiber (CNF-TO) grease demonstrated outstanding lubrication stability across contact loads of 10–40 N and temperatures from 25 to 100 °C, maintaining COF values below 0.1—comparable to the reference LBG at 40 N load. Wear scar analysis confirmed that CNF-based greases significantly reduced wear relative to the lithium reference: CNF-B produced the smallest scar diameter (188 µm at 25 °C) while CNF-TO yielded the lowest at 60 °C (457 µm). (4) Conclusions: Nanofiber type and pretreatment significantly impact the tribological performance of CNF-based biogreases. TEMPO-oxidized CNFs provided stable lubrication under varied loads and temperatures, while all CNFs showed strong thermal adaptability, supporting their use in sustainable lubrication.