Developing　effective　adsorbents　for　wastewater　purification　is　crucial,　as　excessive　emissions　of　toxic　dyes　and　heavy　metal　ions　have　been　proven　harmful　to　ecosystems　and　human　health.　A　NiFe-layered　double　hydroxide/graphitic　porous　carbon　(NiFe-LDH/GPC)　composite　was　fabricated　by　introducing　NiFe-LDH　nanosheets　into　GPC　via　a　simple　hydrothermal　method　to　utilize　the　advantages　of　both　materials　fully,　and　thus　ultimately　obtain　a　composite　adsorbent　with　improved　adsorption　properties.　The　samples　obtained　were　comprehensively　characterized　by　various　characterization　means,　and　the　effects　of　several　critical　influential　factors　on　the　pollutant　uptake　capability　of　the　NiFe-LDH/GPC　were　also　studied　through　batch　experiments.　The　results　show　that　the　as-synthesized　NiFe-LDH/GPC　exhibits　a　three-dimensional　(3D)　fluffy　ultrathin-wall　hierarchical　porous　structure,　which　possesses　a　high　specific　surface　area　and　pore　volume　separately　up　to　506.74　m2/g　and　0.22　cm3　g−1　as　well　as　a　relatively　narrow　pore　size　distribution.　These　characteristics　bring　advantages　to　enhance　the　adsorption　ability　of　the　NiFe-LDH/GPC　for　cationic/anionic　dyes　and　heavy　metal　ions　such　as　congo　red　(CR),　malachite　green　(MG)　and　hexavalent　chrome　(Cr(VI),　which　reached　the　maximum　adsorption　capacity　of　1726.51　mg/g,　1157.11　mg/g　and　155.72　mg/g　under　the　optimum　conditions,　respectively.　Meanwhile,　the　adsorption　behavior　can　be　well　described　by　the　pseudo-second-order　kinetic　model　and　Langmuir　isotherm　model,　reflecting　that　the　sorption　process　mainly　occurred　chemically　in　the　adsorbent　monolayer.　Furthermore,　the　NiFe-LDH/GPC　maintained　relatively　high　adsorption　performance　after　multicycle　testing,　manifesting　its　good　recyclability　and　stability.　©　2024　Elsevier　B.V.