This study reports useful application of the electrokinetic sonic amplitude (ESA) technique in combination with rheometry and electron microscopy techniques for direct probing the stability of low and high-concentrated zirconia (ZrO2) nanosuspensions in the presence of an alkali-free anionic polyelectrolyte dispersant Dolapix CE64. A comparative study of the electrokinetic characteristics and the rheological behavior of concentrated ZrO2 nanosuspensions has been done. Good agreement was obtained from relationship between the electrokinetic characteristics (zeta potential, ESA signal), viscosity, and its pH dependence for each concentrated ZrO2 nanosuspension with different dispersant concentration in the range of 0.9-1.5 mass%. A nanoscale colloidal hypothesis is proposed to illustrate that the addition of different amounts of dispersant influences on both the stability and the electrokinetic and rheological properties of concentrated ZrO2 nanosuspensions. It is found that an optimum amount of 1.4 mass% dispersant at the inherent pH (>9.2) can be attached fully onto the nanoparticles with sufficient electrosteric dispersion effects, suitable for casting applications. Supplementary scanning electron microscopy (SEM) and high-resolution transmission electron microscopy (HR-TEM) analyses followed by colorization effect were taken to verify the visible interaction between dispersant and nanoparticles surfaces. SEM and HR-TEM images proved the existence of visible coverage of dispersant on the surface of individual nanoparticles and showed that thin polyelectrolyte layers were physically bound onto the particles' surfaces. This study will be of interest to materials scientists and engineers who are dealing with dispersion technology, nanoparticle surface treatments, functionalization, characterization, and application of bio/nanoparticle suspensions at various concentrations using different types of polymers.