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Two water-soluble block copolymers composed of acrylic acid (AA), 2-acrylamido-2-methylpropane sulfonic acid (AMPS), and optionally maleic anhydride (MAH) were synthesized through ammonium persulfate-catalyzed free radical polymerization in water. The introduction of aluminum sulfate (AS) into the resulting mixtures significantly reduced the setting times of the paste and enhanced the mechanical strength of the mortar compared to both the additive-free control and experiments facilitated solely by pure AS. This improvement was primarily attributed to the inhibition of rapid Al³⁺ hydrolysis, which was achieved through coordination of the synthesized block copolymers, along with the formation of newly identified hydrolytic intermediates. Notably, the ternary copolymer (AA–AMPS–MAH) exhibited superior performance compared to that of the binary copolymer (AA–AMPS). In the early stages of cement setting, clusters of ettringite (AFt) were found to be immobilized over newly detected linkage phases, including unusual calcium silicate hydrate and epistilbite. In contrast to the well-documented role of polymers in retarding cement hydration, this study presents a novel approach by providing both accelerating and hardening agents for cement setting, which has significant implications for the future design of cement additives.