Melanin nanoparticles (MNPs) are a type of electronegative compound that can be used as photothermal agent for cancer treatment. Nevertheless, the agglomeration of MNP, which is one of the limitations in practice, contributes to the instability of MNP. Pristine layered double hydroxide (LDH), as a kind of positive inorganic material when there exist no other cargo between its layers, can accommodate electronegative molecules between its layers to endow them with stable properties. Hence, in this study, electronegative MNP was intercalated into LDH lamellas via ion-exchange method to obtain the stable original photothermal agent LDH/MNP, solving the tough problem of MNP's agglomeration. The surface morphology, X-ray diffraction and fourier transform infrared spectra affirmed the successful intercalation of MNP between LDH lamellas. The Z-average particle sizes of LDH/MNP on day 0, 7 and 14 were measured as 221.8 nm, 227.6 nm and 230.5 nm without obvious fluctuation, while the particle sizes of MNP went through dramatic enlargement from 105.8 nm (day 0) to 856.1 nm (day 7), indicating the better stability of LDH/MNP than MNP. The typical polymer dispersity index (PDI) values on day 0, 7 and 14 verified the better stability of LDH/MNP, too. Photothermal properties of LDH/MNP were assessed and the results ensured the representative photothermal properties of LDH/MNP. The fine cytocompatibility of LDH/MNP was verified via cytotoxicity test. Results confirmed that the agglomeration of MNP disappeared after its intercalation into LDH and LDH/MNP possessed fine stability as well as typical photothermal property. The intercalation of MNP into LDH gave the photothermal agent MNP a promising way for its better stability and long-term availability in photothermal treatment.