Oxygen-containingdefectsareveryimportantforalteringthenonlinearoptical(NLO)propertiesofgraphene.Toinvestigatethecorrelationbetweenoxygen-containingdefectsandthesynergisticNLOresponseingraphenebasednanocomposites,weattachedCdSnanocrystalsonthesurfaceofgraphene(G)andpreparedG/CdSnanohybrids(NHs)consistingofvariousoxygen-containingfunctionalgroupsviaachemicalmethod.TheNLOabsorptionandrefractionofG/CdSNHsundersinglepulselaserirradiationareenhancedby10.8timeswiththeconcentrationdecreaseofsurfaceoxygen-containinggroups,whichmightbeattributedtothelocalfieldeffectsandsynergeticeffectsstemmingfromchargetransferbetweenthetwocomponents.However,theopticalnonlinearityisdecreasedwithfurtherconcentrationdecrease,whichmightarisefromsp~2fragmentinterconnectionandsurfacedefectsintheNHs.TheNLOabsorptiontransformationfromtwo-photonabsorptiontosaturableabsorptionwithoxygendecreaseisobserved,andintensity-relatedNLOabsorptionandrefractioninNHsarealsodiscussed.Meanwhile,theG/CdSNHsexhibitsuperiorNLOproperties,implyingpotentialapplicationsofNHmaterialinNLOdevices.