A simple and facile approach has been applied for the synthesis of molybdenum disulfide nanosheets (MNs). Molybdenum disulfide nanosheets were prepared by mix‐solvent reflux exfoliation technique of bulk MoS2 with ethanol/water as the solvent. In this paper, a novel nano sorbent is reported for the surface grafting of poly [N‐Vinyl caprolactam‐co‐Vinyl Acetate] copolymer onto molybdenum disulfide nanosheets. The MNs@ p (NVCL‐co‐VAc) was modified by 3, 4‐diaminobenzoic acid (DABA) to enhance its adsorption capacity. The ability of MNs@ p (NVCL‐co‐VAc)‐DABA was estimated as a nanocarrier for the delivery of Imatinib Mesylate (IM) as an anticancer drug. The polymer grafted MNs@ p (NVCL‐co‐VAc)‐DABA was characterized by using field emission scanning electron microscopy, Fourier transform infrared spectroscopy, thermogravimetric analysis, elemental analysis, and X‐ray powder diffraction. The effect of the experimental parameters, such as pH, contact time, and the temperature was evaluated. In vitro controlled drug release and phototherapy under near‐infrared (NIR) light irradiation are also discussed. In vitro release of IM from IM/MNs@ p (NVCL‐co‐VAc)‐DABA nanocarriers in the simulated blood fluid (pH = 7.4) shown that the release of IM was faster at 50°C than that at 37°C. The drug release amount under NIR light irradiation reached up to 98% over 15 min, which was about 12 times that without NIR light irradiation. The existence of absorbed NIR energy causes shrinkage of thermosensitive polymer chains and successfully caused the drug release. The sorption process was described by the Langmuir model and pseudo‐second‐order kinetic. The drug release kinetics was examined using Zero‐order, First‐order, Korsmeyer–Peppas, and Higuchi mathematical models.