Cellulose nanofibril (CNF) is a type of nano-sized cellulosic material with a high aspect ratio and a large specific surface area, which makes it a promising additive to flocculate particles such as fillers. In this study, CNFs were prepared by wet disk-milling with three different degrees of fibrillation. The effect of the CNF on the flocculation of precipitated calcium carbonate (PCC) was elucidated. A photometric dispersion analyzer (PDA) investigated the flocculation phenomena resulting from the interactions between the PCC and the CNF, or polymers, in real-time. The results clearly showed that CNF could be used to control the flocculation behavior of the PCC particles. Scanning electron microscopy (SEM) images showed that the CNFs functioned as bridges between the two PCC particles. A significant reflocculation capability was observed in one- and two-component systems that consisted of CNFs. The addition of cationic starch (C-starch) could induce more efficient flocculation within a two-component system.