Cellulose nanofibrils, which attract extensive attention as a bio-based, sustainable, high-performance nanofibril, are believed to be predominantly hydrophilic. This study aimed to prove the presence of an amphiphilic "Janus-type fiber surface" in water with hydrophobic and hydrophilic faces in a cellulose nanofibril (ACC-CNF) that was prepared by the aqueous counter collision method. We clarified the surface characteristics of the ACC-CNF by confocal laser scanning microscopy with a carbohydrate-binding module and congo red probes for the hydrophobic planes on the cellulose fiber surfaces and calcofluor white as hydrophilic plane probes. The results indicated the presence of both characteristic planes on a single ACC-CNF surface, which verifies an amphiphilic Janus-type structure. Both hydrophobic probes adsorbed onto ACC-CNFs for the quantitative evaluation of the degree of ACC-CNF surface hydrophobicity by Langmuir's adsorption theory based on the optimal maximum adsorption amounts for various starting raw material types.