Cationic polyacrylamides (C-PAMs) have been widely used as flocculating agents to aggregate particles carrying negatively charged surfaces. This study examined the effects of hydrolysis of C-PAM on its adsorption behaviour and flocculation of negatively charged particles, specifically ground calcium carbonate (GCC). C-PAM hydrolysis was examined using polyelectrolyte titration and ion chromatography, while the adsorption behaviour of the polymer was monitored using a quartz crystal microbalance with dissipation (QCM-D). Laser diffraction spectroscopy was used to measure the size of the GCC aggregates under neutral and alkaline conditions. The charge density measurements and ion chromatograms indicated that the hydrolysis of C-PAM was accelerated with increased pH and temperature. The QCM-D measurements of hydrolysed C-PAMs, adsorbed on a substrate with a flat and rigid structure indicated that hydrolysis of C-PAM suppressed its ability to cause inter-particle bridging flocculation, which reduced the aggregate size of GCC.