In this paper, a microparticle system consisting of cationic polyacrylamide (CPAM) and anionic spherical polyelectrolyte brushes (ASPB) is proposed to improve the retention of pulp suspension containing bleached reed kraft pulp and precipitated calcium carbonate (PCC). We first describe the preparation of ASPB. The ASPB, consisting of a carbon sphere (CS) core and a shell of sodium polystyrene sulfonate (PSSNa) brushes, was synthesized by surface-initiated polymerization. The structure and morphology of ASPB were characterized by Fourier-transform infrared spectrometry (FTIR), field emission scanning electron microscopy (FESEM) and transmission electron microscopy (TEM). Then, flocculation and retention of pulp suspension by a CPAM/ASPB dual-component system were examined. Our results indicate that more highly effective flocculation and higher retention efficiency could be achieved simultaneously by a CPAM/ASPB dual-component system when compared to the conventional microparticle system. Bridging flocculation and electrostatic attraction might be the main flocculation mechanism for CPAM/ASPB systems.