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The effects of a polyelectrolyte dispersant agent, polyethyleneimine (PEI), on the rheology of zirconia 3Y-TZP suspensions and the densification characteristics of sintered zirconia were investigated. The colloidal processing technique was used to minimize the agglomeration of nanoparticles during the fabrication of the samples. Five batches of 10% zirconia suspensions containing different amounts of PEI at 0.3, 0.4, 0.5, 0.6, and 0.7 wt% were prepared. The rheological properties of the zirconia suspensions were determined using a rotational viscometer. The optimum amount of PEI that can maximize powders dispersion was determined. The green samples were then prepared using the slip casting process. The samples were densely sintered at a final sintering temperature of 1300 °C. The result revealed that the zirconia suspension with 0.5 wt% PEI was the most optimum amount to obtain a well-dispersed suspension. The sintered density of zirconia 3Y-TZP reached its maximum by adding 0.5 wt% PEI.