Sediments polluted with hydrophobic organic contaminants (HOCs) and metals can pose environmental risks, yet effective remediation remains a challenge. We investigated a new composite sorbent comprising granular activated carbon (GAC) and a calcium-silicate (Polonite®, PO) for thin-layer capping of polluted sediment, with the aim to sequester both HOCs and metals. Box cores were collected in polluted Oskarshamn harbor, Sweden, and the sediments were treated with GAC and/or Polonite in a 10-week mesocosm study to measure endpoints ranging from contaminant immobilization to ecological side effects on native fauna and biogeochemical processes. The GAC particle size was 300–500 μm to reduce negative effects on benthic fauna (by being non-ingestible) and of biogenic origin (coconut) to have a small carbon footprint compared with traditional fossil ACs. The calcium-silicate was a fine-grained industrial by-product used to target metals and as a carrier for GAC to improve the cap integrity.GAC decreased the uptake of dioxins (PCDD/Fs) in the bivalve Macoma balthica by 47 % and the in vitro bioavailability of PCB by 40 %. The composite cap of GAC + Polonite decreased sediment-to-water release of Pb < Cu < Ni < Zn < Cd by 42–98 % (lowest to highest decrease) and bioaccumulation of Cd < Zn < Cu in the worm Hediste diversicolor by 50–65 %. Additionally, in vitro bioavailability of Pb < Cu < Zn, measured using digestive fluid extraction, decreased by 43–83 %.GAC showed no adverse effects on benthic fauna while Polonite caused short-term adverse effects on fauna diversity and abundance, partly due to its cohesiveness, which, in turn, can improve the cap integrity in situ. Fauna later recovered and bioturbated the cap. Both sorbents influenced biogeochemical processes; GAC sorbed ammonium, Polonite decreased respiration, and both sorbents reduced denitrification. In conclusion, the side effects were relatively mild, and the cap decreased the release and bioavailability of both HOCs and metals effectively, thus offering a promising sustainable and cost-effective solution to remediating polluted sediments.