In this work, electrospun fibrous membranes based on the polycaprolactone (PCL)/polyethylene oxide (PEO) blended with pure, 3-Aminopropyltriethoxysilane (APTES) or 3-Glycidoxypropyltrimethoxysilane (GPTMS) modified halloysite nanotubes (HNT) were prepared by electrospinning for curcumin (Cur) delivery system. The morphological and physicochemical properties of the fabricated membranes were characterized by scanning electron microscopy (SEM), atomic force microscopy (AFM), Fourier transform infrared spectroscopy (FTIR), and X-ray diffraction (XRD). In vitro release of from the Cur loaded fibrous membranes was examined in simulated physiological condition by ultraviolet-visible spectroscopy. Besides, in vitro cytotoxicity on the MCF-7 breast carcinoma cells was evaluated. The results demonstrated that the silane-modified HNTs (HNT-APTES and HNT-GPTMS) displayed a much higher Cur loading capacity while APTES modified HNT had the maximum encapsulation efficiency. Moreover, in vitro Cur release studies demonstrated that PCL/PEO-Cur/HNT-APTES membrane has a slower release profile. The release mechanism of Cur from all membranes was fitted by the Peppas-Sahlin kinetic model indicating a pseudo-Fickian and non-Fickian release. Additionally, the PCL/PEO-Cur/HNT-APTES membrane showed the highest toxicity against MCF-7 breast cancer cells. In conclusion, the uses of this Cur loaded PCL/PEO electrospun fibrous membranes blended with the APTES modified HNT can be used to loading of other drugs for controlled drug delivery system, especially as an anticancer carrier.