The invention relates to preparation of Fe/Co-NPS co-doped porous carbon microspheres and application of the Fe/Co-NPS co-doped porous carbon microspheres in removal of organic pollutants. The preparation method disclosed by the invention comprises the following steps: synthesizing Fe3O4 magnetic microspheres by adopting a solvothermal method; synthesizing Fe3o4@PZS core-shell microspheres by taking the Fe3O4 magnetic microspheres as a nucleus and adopting a hard template method; generating a ZIF-67 shell layer by using an in-situ growth method; carbonizing and acidulating a sample to finally obtain the Fe/Co-NPS co-doped porous carbon microspheres. The prepared porous microspheres have the advantages of relatively-large specific surface area and relatively-high porosity; in addition, adsorption and degradation of multiple organic pollutants can be quickly realized by catalyzing; the porous microspheres can be recycled by magnets.