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Cellulose nanocrystal (CNC)-based materials display apparently erratic wetting behaviors with contact angle (CA) variations as large as 30° from sample to sample. This work hypothesizes that it is the orientation of CNC amphiphilic functionalities at the interface with air that causes the variability in CA. By exploiting relationships with the Hansen solubility parameter theory, a set of surface tension parameters is proposed for both the polar and the non-polar surfaces of cellulose I_β nanocrystals. These coefficients elucidate the wettability of CNC materials by establishing a correlation between the wetting properties of the air/sample interface and its chemical composition in terms of non-polar moieties. Advancing/receding CA experiments suggest that, while spin-coating CNC suspensions yield purely polar films, oven-casting them produces amphiphilic surfaces. We proposed a mechanism where the state of …