Core-shell nanocomposites are one of the most important achievements in the fast-growing field of nanotechnology. The combination of multi-responsive nano-shell with luminescent and photothermal core has led to promising applications in various fields such as optics, electronics and medicine. In this work, a nanosized core-shell system composed by carbonized dots core and poly(N-isopropylacrylamide) shell was developed and the photothermal triggered release of doxorubicin was demonstrated. The system was fully characterized by H1-NMR, DLS, Z-potential, AFM, optical absorption and fluorescence measurements. A photothermal conversion efficiency (η) value of about 67.9% and a doxorubicin photo-release rate value of about 1.0% min−1 were measured. Molecular dynamic (MD) simulations data were in agreement with experimental results, at 310 K the coil-to-globule transition and a consequent desorption of doxorubicin from the polymer were observed. Both the radius of gyration and the fluctuation of the distance doxorubicin-PNIPAM pointed that the temperature above the LCST and the acid pH facilitated the polymer transition. Moreover, MD simulations and experimental data suggested an influence on the lower critical solution temperature (LCST) exerted by the number of polymer chains anchored to the carbon core.