The present paper aimed to synthesize, using thermal-treatment method, a variety of Co1-XZnxFe2O4-based nanocarriers (NCs) as Dual-controlled and targeted drug delivery systems (DDS) and provide a new structure as NCs suitable for the loading and pH-responsive characteristics of the chemotherapeutic curcumin (CUR). To study the structure, surface morphology, surface charge and magnetic properties of NCs, X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), transmission electron microscopy (TEM), Zetasizer and vibrating sample magnetometer (VSM) were applied here. TEM images of Co0.2Zn0.8Fe2O4 (Co-0.2) showed that NCs had a uniform spherical mesoporous morphology with an average grain size of about ∼17 nm. Also, it was found that Drug loading was very high, about 22.70 and 21.99 for Co0.6Zn0.4Fe2O4 (Co-0.6) and Co0.4Zn0.6Fe2O4 (Co-0.4), respectively. As indicated, NCs had highly pH-dependent drug release behavior, although different and unique in every one of them, which could be related to zeta potential of Co-0.6. In fact, the neutral zeta potential of Co-0.6 became positivewhen the pHof releasingmedia changed from7.4 to 5.5. Consequently, the hydrogen bond between the Co-0.6 and CUR brake. Therefore, as expected, drug releasing varied from Co-0.6 to about 54% at pH 5.5, rather 29% at pH 7.4. To determine the cytotoxicity of NCs, hemolysis assay, MTT assay and acute toxicity test were used. The tests showed that NCs had the least in vitro and in vivo cytotoxicity and NCs, as a result, could be regarded to be nontoxic. MTT results demonstrated that drug loaded NCs had the same cell viability as bare drugs. Then, it can be concluded that these NCs have the potential required to act as drug delivery systems for anti-cancer drugs delivery such as CUR.