The present paper describes a downsizing mechanism of an aqueous counter collision (ACC) process that enables the rapid preparation of cellulose nanofibrils (CNFs) as an aqueous dispersion solely by impinging a pair of water jets containing the raw materials. Extensive studies have revealed that the resulting CNFs by ACC have amphiphilic fiber surfaces, in which two kinds of faces with different natures are present along the entire fiber axis. They therefore have superior adsorption to surfaces of various conventional polymer plastics. These characteristic adsorption behaviors, which are totally different from those for other CNFs prepared by other means, are attributable to their hydrophobic surfaces. In the present study, high-resolution microscopy, including atomic force microscopy, confocal laser scanning microscopy, and scanning electron microscopy with broad argon ion beam milling, was used to determine how the emergence of such hydrophobic characteristics in a nanofibril face occurs in relation to the ACC nanopulverization mechanism due to the collision of the pair of water jets.