Electrospun nanofibers (NFs)‐based drug delivery approaches are of particular interest as a hopeful implantable nanoplatform for localized cancer therapy and treating tissue defect after resection, allowing the on‐site drug delivery with minimal side effect to healthy cells. To maintain therapeutic concentrations of anticancer molecules for a relatively long time through a combination of burst and sustained drug release mechanisms, a hybrid of polycaprolactone and gelatin (PCL/GEL) was used for co‐encapsulation of free curcumin (CUR) and CUR‐loaded mesoporous silica nanoparticles (CUR@MSNs) via electrospinning, resulting in a novel drug‐loaded nanofibrous scaffold, CUR/CUR@MSNs‐NFs. The as‐prepared MSNs and composite NFs were characterized via TGA, FTIR, FE‐SEM, TEM, and BET. In vitro release profile of CUR from CUR/CUR@MSNs‐NFs was examined, and the in vitro antitumor efficacy against MDA‐MB‐231 breast cancer cells was also evaluated through MTT, scratch assay, DAPI staining, and real‐time PCR. The results disclosed that the smooth, bead‐free, and randomly oriented CUR/CUR@MSNs‐NFs displayed a combination of initial rapid discharge and sustained release for CUR, which led to higher cytotoxicity, lower migration as well as a more pronounced effect on apoptosis induction than CUR‐NFs and CUR@MSNs‐NFs. The present study illustrated that the dual drug release mechanisms through MSN/NF‐mediated drug delivery systems might have a highly hopeful application as a localized implantable scaffold for potential postoperative breast cancer therapy.

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