Charging and aggregation processes of titania nanosheets (TNS) were extensively studied in the presence of oppositely charged or like-charged polyelectrolytes in aqueous dispersions. The surface charge of the TNS was systematically varied by the pH; therefore, positive nanosheets were obtained at pH 4 and negative ones at pH 10. Strong adsorption of poly(styrene sulfonate) (PSS) of high negative line charge density on the TNS was observed at pH 4, leading to charge neutralization and reversal of the original sign of charge of the nanosheets. The adsorption of like-charged poly(diallyldimethylammonium chloride) (PDADMAC) was also feasible through a hydrophobic interaction. The predominating interparticle forces were mainly of the DLVO-type, but additional patch-charge attraction also took place in the case of PSS at low surface coverage. The TNS was found to be hydrophilic at pH 10 and no adsorption of like-charged PSS was possible because of strong electrostatic repulsion between the polyelectrolyte and the surface. The PDADMAC showed high affinity to the oppositely charged TNS surface in alkaline dispersions, giving rise to neutral and positively charged nanosheets at appropriate polyelectrolyte doses. Formation of a saturated PDADMAC layer on the TNS led to high resistance against salt-induced aggregation through the electrosteric stabilization mechanism. These results shed light on the importance of polyelectrolyte concentration, ionic strength, and charge balance on the colloidal stability of TNS, which is especially important in applications, where the nanosheets are dispersed in complex solution containing polymeric compounds and electrolytes.