Heavy metal cations and anions contaminated groundwater was a big challenge to water resource safety. Herein, a green sulfidated micro zero-valent iron-based hydrogel (SA-S-mZVI) was synthesized using sodium alginate biomass for the simultaneous removal of heavy metal cations (Cu(II), Pb(II), Cd(II)) and anions (Cr(VI)). The sulfur modification and incorporation of sodium alginate hydrogel facilitated the efficient and sustainable removal of both single and multi-heavy metals. The co-existing heavy metal cations benefited the removal of Cr(VI), and heavy metals were mostly transformed into stable precipitates. The presence of organic substance and ions slightly affected the removal of heavy metals. Long-term column experiments (240 days) showed that SA-S-mZVI maintained over 99.9 % removal efficiency for heavy metal cations and anions, without adverse impacts on the groundwater environment. This study provided new insights into the development of eco-friendly, long-lasting zero-valent iron-based hydrogels for in-situ remediation of heavy metals-contaminated groundwater.