Iron(III) bis(phenol) amine complex immobilized on the surface of functionalized graphene oxide nanosheets (FeLGDC‐AP/GO) has introduced as a highly active and recoverable catalyst for the epoxidation of alkenes. Optimizing different parameters in the oxidation of styrene as a model substrate revealed that 100% conversion and selectivity were obtained toward styrene oxide in the presence of H2O2 (28 wt%) as oxidant and water/acetone (3:1) as a solvent system in a bicarbonate buffer system. Furthermore, the catalyst displayed 54%–100% conversion and 90%–100% selectivity for the epoxidation of various aromatic and aliphatic alkenes under optimized reaction conditions at room temperature. The recycling experiment showed that FeLGDC‐AP/GO could be easily recovered by simple filtration and recycled six times without loss of the activity and selectivity. The high catalytic activity and selectivity of the developed catalyst could be attributed to the well‐designed coordination sphere around the iron core as well as the presence of GO support, which facilitates the electron transfer process beside the catalyst recovery.