To improve the dewatering performances of the waste slurry, a new Fe-Polyacrylamide (Fe-PAM) flocculant was synthesized. Comparative analysis with various ionic forms of polyacrylamide (PAM) reveals that the Fe-PAM flocculant has the shortest flocculation time, the lowest optimal shear gradient for flocculation, and the best filtration performance. The capillary suction time (CST) of Fe-PAM treated slurry was improved from 262.3 s (raw sample) to 6.0 s. Moreover, sludge treated with Fe-PAM exhibits the lowest porosity under the same consolidation pressure and the highest permeability at the same void ratio. In addition, mercury intrusion porosimetry (MIP) results indicated that the Fe-PAM-treated sample features the highest number of largesized inter-aggregate pores (average value of 184.2 nm and median value of 23.2 nm) and the greatest pore connectivity (60.55 %), contributing to its superior permeability. The effectiveness of Fe-PAM is further elaborated through a synergistic flocculation mechanism, encompassing the electrical neutralization effect of the inorganic metal Fe3+ and the adsorption bridging effect of PAM's long-chains. This study demonstrates the potential of the synthesized Fe-PAM flocculant to enhance the dewatering efficiency of high-water content slurry and offers valuable insights for synthesizing advanced flocculants in slurry treatment engineering.