Efficient activation of peroxydisulfate (PDS, SO) was achieved in this study by a hybrid of reduced graphene oxide (rGO) and layered double hydroxide (LDH). The peroxydisulfate was intercalated into the interlayers of LDH that was combined with rGO. This sample contributed to 92.4 % of phenol (PhOH) removal at 25 °C with a PDS loading amount of 0.4 mmol/g, which is better than its LDH-PDS counterpart. A high activation of PDS in rGO/LDH-PDS was also observed during the oxidation of 4-bromophenol (4-BrPhOH), 2,4-dibromophenol (2, 4-BrPhOH), 2,6-dibromophenol (2, 6-BrPhOH) and bisphenol A (BPA). As a redox reaction of PDS in LDH, this result determined that the composite of rGO/LDH caused more PDS to be activated than LDH. As the defective rGO sites activated the PDS on the surface or edges of LDH layers, the breaking of the OO bond in PDS generated SO radicals from intercalated peroxydisulfate. This result was supported by the radical scavenger experiment, electron paramagnetic resonance measurements, and the increased number of oxygen functional groups in the reacted rGO. Our work thus provided a novel strategy for PDS activation to use in environmental remediation.