Nanocomposites are promising drug carriers to treat terminal cancers with few adverse effects. Herein, nanocomposite hydrogels composed of carboxymethyl cellulose (CMC)/starch/reduced graphene oxide (RGO) were synthesized via a green chemistry approach and then encapsulated in double nanoemulsions to act as pH-responsive delivery systems for curcumin, a potential antitumor drug. A water/oil/water nanoemulsion containing bitter almond oil served as a membrane surrounding the nanocarrier to control drug release. DLS and zeta potential measurements were used to estimate the size and confirm the stability of curcumin-loaded nanocarriers. The intermolecular interactions, crystalline structure and morphology of the nanocarriers were analyzed through FTIR spectroscopy, XRD and FESEM, respectively. The drug loading and entrapment efficiencies were significantly improved compared to previously reported curcumin delivery systems. In vitro release experiments demonstrated the pH-responsiveness of the nanocarriers and the faster curcumin release at a lower pH. The MTT assay revealed the increased toxicity of the nanocomposites against MCF-7 cancer cells compared to CMC, CMC/RGO or free curcumin. Apoptosis was detected in MCF-7 cells via flow cytometry tests. The results obtained herein support that the developed nanocarriers are stable, uniform and effective delivery systems for a sustained and pH-sensitive curcumin release.