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This study aims to investigate workability and microstructural characteristics of sodium hexametaphosphate (SHMP)-treated calcium bentonite (Ca-bentonite) as a potential material for soil–bentonite slurry trench cutoff walls. First, a series of Marsh viscosity, filtrate loss, density, and pH experiments are performed on bentonite – tap water slurries containing Ca-bentonite amended with 0%–8% SHMP dosages. Subsequently, scanning electron microscopy (SEM), X-ray diffraction (XRD), Fourier transform infrared spectroscopy, and zeta potential tests are conducted to explore microstructural characteristics that control the mechanisms of SHMP treatment. The results indicate that the workability of the slurry is significantly improved with SHMP addition. The SEM, XRD, and zeta potential analyses show that SHMP-amended Ca-bentonite possesses a more dispersed structure and higher negative zeta potential relative to the unamended Ca-bentonite. The mechanisms of SHMP amendment are identified to be exchange of bivalent calcium cations in Ca-bentonite by monovalent sodium cations in the SHMP, sorption of the SHMP anions that give the clay system a steric stabilization and increased negative surface charge density, and sequestration of the bivalent calcium cations on the Ca-bentonite. Overall, the SHMP treatment is effective in making the Ca-bentonite slurry amenable for use in the soil–bentonite slurry trench wall construction.