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An optimal methodology to accurately determine the dimensions of CNCs was developed using atomic force microscopy and small-angle X-ray scattering techniques. The thermodynamics of interactions of CNCs with cationic counterions was studied with isothermal titration calorimetry, and were found to be dependent on the hydration characteristics of the counterion. The dynamic behaviour of CNCs in the presence of salts was investigated using multi-angle depolarized dynamic light scattering, and was found to be dependent on size polydispersity of the particles and - to a lesser extent - on the mechanism of the counterion adsorption. The phase behaviour of CNCs varying by their source (cotton and bacterial CNCs) and surface chemical functional groups (sulfate, carboxylate and both) was studied subsequently by polarization imaging, particle-tracking microrheology, and small-angle X-ray scattering. The competition of isotropic-nematic phase separation and ion-induced gelling was studied in the presence of various monovalent counterions, and "CNC concentration - ionic strength" phase diagrams were determined.