To overcome the shortcomings of existing Fenton catalysts, such as secondary contamination caused by iron-containing sludge, harsh pH acidic conditions, poor recovery and recycling performance, and difficult separation, an Fe-loaded geopolymer microsphere (Fe-GLM) with a high specific surface area (68.5 m2/g), pore volume (0.0596 cm3/g), and excellent Fenton catalytic performance was prepared in this paper for dye wastewater treatment. Degradation experiments for organic dye wastewater show that the degradation ability and morphological structure of Fe-GLM does not change after multiple cycles, achieving a degradation and removal rate of more than 99%. Fe-GLM can be used to degrade both anionic dye and cationic dye wastewater in the pH range of 2–10 showing excellent catalytic performance.