Sustainable utilization and development for contaminated mudflat sites face dual challenges associated with contaminant enrichment and engineering diseases, impacting ecological quality and coastal construction. Commonly used cement has limitations in ensuring geo-environmental engineering performances for polluted sediments. This study investigates a solidification/stabilization approach using novel chitosan-enhanced alkali-activated material (CTS-AAM) to remediate highly concentrated zinc-contaminated sediments. Results exhibit that the compressive strength and water stability of sediments are remarkably improved by CTS-AAM, satisfying engineering service even under long-term immersion and zinc accumulation. Significant improvements dependent on curing period and CTS-AAM dosage also reflect in the resistance to deformation of remediated sediments, maintaining low-compressibility states due to the enhancement of structural yield stress. The leaching toxicity of remediated sediments meets Zn ≤ 5.0 mg/L, as zinc primarily distributes to the residual fraction associated with low mobility. The bidirectional enhancement of toxic sediment is attributed to the generation of hydrates with cementitious and pore-filling effects through hydration reactions. Simultaneously, chitosan with hydrated gels and ettringite collectively form gel networks and compact skeleton structures within sediments, as well as immobilize Zn through comprehensive physical encapsulation, chemical binding, and chelation. This study provides a feasible strategy for future projects involving remediation and utilization of mudflats.