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The design and development of multifunctional nanoparticles have attracted great interest in biomedical research. This study aims to prepare pH-responsive melanin-like nanoparticles for T1-weighted magnetic resonance imaging (MRI) and photothermal therapy. The new multifunctional nanoparticles (amino-Fe-PDANPs) are synthesized by copolymerization of dopamine and its derivative amino-N-[2-(diethylamino) ethyl]-3,4-dihydroxy-benzenepropanamide (N-Dopa) at room temperature. The size of nanoparticles can be controlled by NaOH concentration. The incorporation of N-Dopa is characterized by NMR and FT-IR. From transmission electron microscopy (TEM), the nanoparticles exhibit excellent dispersion stability in water and are spherical in shape. The MRI measurement has demonstrated that amino-Fe-PDANPs have a significant signal enhancement in responding to the acidic solution. Confirmed by the photothermal study, the nanoparticles exhibit a high photothermal conversion efficiency. The melanin-like multifunctional nanoparticles integrate both diagnosis and therapeutic functionalities, indicating the potential for theranostic application.