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Recently, utilizing biomass to synthesize novel functional materials has been a focus of significant interests in a myriad of fields such as environmental remediation. Herein, Ca–Fe–O porous materials were successfully synthesized by utilizing oyster shells and K2FeO4 according to a simple one-pot method. According to the result of TEM, Fe3O4 was obtained by reducing K2FeO4 and then deposited in situ on the Ca(OH)2 nanosheets derived by CaO precursor. Such Ca–Fe–O porous materials showing outstanding adsorption capacity for RhB (146.11mg/g) and MB (135.70mg/g), additionally, would generate abundant H2O2 and remove the organic compounds through a Fenton-like reaction. It is hoped that our work could spur further interest in utilizing biomass to rationally design a variety of promising functional materials for environmental remediation.