This study tested two sediment amendments with active sorbents: injection of aluminum (Al) into sediments and thin-layer capping with Polonite (calcium-silicate), with and without the addition of activated carbon (AC), for their simultaneous sequestration of sediment phosphorus (P), hydrophobic organic contaminants (HOCs), and metals. Sediment cores were collected from a eutrophic and polluted brackish water bay in Sweden and incubated in the laboratory to measure sediment-to-water contaminant release and effects on biogeochemical processes. We used diffusive gradients in thin-film passive samplers for metals and semi-permeable membrane devices for the HOC polychlorinated biphenyls and polycyclic aromatic hydrocarbons. Al injection into anoxic sediments completely stopped the release of P and reduced the release of cadmium (Cd, -97%) and zinc (Zn, -95%) but increased the sediment fluxes of PAH (+49%), compared to the untreated sediment. Polonite mixed with AC reduced the release of P (-70%), Cd (-67%), and Zn (-89%) but increased methane (CH4) release. Adding AC to the Al or Polonite reduced the release of HOCs by 40% in both treatments. These results not only demonstrate the potential of innovative remediation techniques using composite sorbent amendments but also highlight the need to assess possible ecological side effects on, for example, sedimentary microbial processes.