Sediments contaminated with hazardous metals pose risks to humans and wildlife, yet viable management options are scarce. In a series of laboratory experiments, we characterized Polonite® – an activated calcium-silicate – as a novel sorbent for thin-layer capping of metal-contaminated sediments. We tested a fine-grained by-product from the Polonite production as a cheap and sustainable sorbent. First, Polonite was reacted with solutions of Cu, Pb, and Zn, and the surface chemistry of the Polonite was examined using, e.g., scanning electron microscopy to investigate metal sorption mechanisms. Batch experiments were conducted by adding Polonite to industrially contaminated harbor sediment to determine sorption kinetics and isotherms. Importantly, we measured if the Polonite could reduce metal bioavailability to sediment fauna by performing digestive fluid extraction (DFE). Finally, a cap placement technique was studied by applying a Polonite slurry in sedimentation columns. The results showed rapid metal sorption to Polonite via several mechanisms, including hydroxide and carbonate precipitation, and complexation with metal oxides on the Polonite surface. Isotherm data revealed that the sediment uptake capacity (Kf) for Cu, Pb, and Zn increased by a factor of 25, 21, and 14, respectively, after addition of 5% Polonite. The bioavailability of Cu, Pb, and Zn was reduced by 70%, 65%, and 54%, respectively, after a 25% Polonite addition. In conclusion, we propose that sediment treatment with low doses of the Polonite by-product can be a cheap, sustainable, and effective remediation method compared to other more intrusive methods such as dredging or conventional isolation capping.