Conventional subsurface barrier materials for contamination containment deteriorate in aggressive environments and only have a limited exchange/adsorption capacity for heavy metals. This study focused on the potential use of superabsorbent polymer (SAP) in soil-cement subsurface barriers for enhanced heavy metal sorption and self-healing. The SAP adsorption results for lead, copper, zinc and nickel were well fitted by the Langmuir model. The SAP had the highest adsorption capacity for lead at 175 mg/g, and plays a key role in the removal of the heavy metals in an acidic environment. In addition, the incorporation of SAP in soil-cement increased the ductility and had negligible adverse effects on mechanical and permeability properties. When cracks propagate in the matrix, the SAP is exposed to the ingress of water and swells, and this swelling reaction seals the cracks. The SAP-containing soil-cement demonstrated enhanced self-healing performance in terms of the recovery of permeability. The uniform dispersion and the 3D network of the SAP were observed using micro-CT scanning, and good bonding and self-healing mechanism were confirmed by SEM-EDX analysis. The results suggest the significant potential for the SAP-based approach for the development of more resilient subsurface barriers with enhanced heavy metal sorption and self-healing.