The physical and chemical properties of cellulose nanocrystals (CNC) were regulated by physical crosslinking with chitosan particles (CSp). At a fixed concentration (0.5 wt%) of CNC, varying CSp concentration (0.02-0.5 wt %) influenced the morphologies and chemical properties of the obtained complex particles (CNC-CSp). The results of Fourier transform infrared spectroscopy (FTIR) and zeta potential confirmed the electrostatic and hydrogen bonding interactions between CSp and CNC. At a low CSp concentration (0.02-0.05 wt%), the charge shielding effect induced the formation of particle aggregation networks, thus showing increased viscosity, turbidity and size (153.4-2605.7 nm). At a higher CSp concentration (0.1-0.5 wt%), the hydrogen bonding interaction promoted CSp adsorption onto the surface of CNC, thus facilitating the dispersion of CNC-CSp due to electrostatic repulsion caused by surface-adsorbed CSp. In addition, CSp improved the thermal stability, hydrophobicity (41.87-60.02.) and rheological properties of CNC. Compared with CNC, CNC-CSp displayed a better emulsifying ability and emulsion stability, in which CSp could play a dual role (i.e., charge regulator and stabilizer). This study suggests that introducing CSp can improve the properties and application potentials of CNC as food colloids.