The major limitations of traditional methods of anticancer drug delivery include systemic distribution and frequent administration intravenously. To address these issues, in our present approach, we have fabricated a nano hybrid silk hydrogel system for localized, targeted, and on-demand delivery of anticancer drugs. The hybrid system contains a blend of two varieties of silk protein and doxorubicin (DOX)-loaded folic acid functionalized single-walled carbon nanotubes (SWCNT-FA/DOX). Owing to the single-walled carbon nanotube (SWCNT) incorporation, the mechanical strength of the hybrid silk hydrogel composite enhanced significantly. A slow and sustained DOX release was recorded over a 14 day study. The amount of DOX released was determined by concentration of the SWCNT-FA/DOX payload, rate of silk degradation, pH of the released medium, and incubation temperature. The intermittent exposure of near-infrared light to the hybrid gel system stimulated on-demand DOX release. The studies demonstrated the active targeting of SWCNT-FA/DOX to folic acid receptor-positive (FR) cancer cells. The silk hydrogel, being viscoelastic in nature, is easily injectable to the targeted site. Hence, the developed silk hybrid gel system may allow its near or intratumoral implantation, where it may act as a depot for anticancer drug-loaded nanoparticles. The sustained, targeted, and external-stimuli-dependent DOX released at the localized tumor site is expected to reduce its systemic side effects and show an efficient way to treat the cancer.