Laryngeal cancer is highly aggressive and insensitive to conventional targeted therapies, which often result in poor therapeutic outcomes. Image-guided precision therapy is a promising strategy in oncology that has superior safety and efficacy versus conventional therapies. Here, we present a multifunctional theranostic nanoplatform based on melanin-coated gold nanorod (GNR) that exhibits excellent multimodal imaging ability and photothermal effects. These attributes make the platform applicable for multimodal photoacoustic (PA)/positron emission tomography (PET)/magnetic resonance (MR) image-guided photothermal treatment of laryngeal cancer. The melanin nanoparticles markedly suppress the cytotoxicity of the template cetyltrimethylammonium bromide bilayer and conferred the GNR with excellent PET/MR imaging performances, due to their native biocompatibilities and strong affinities to metal ions. Moreover, the introduction of GNR to the melanin nanoparticles greatly improved the near-infrared absorbances and passive targeting capabilities, leading to exceptional PA imaging and photothermal ablation of tumors. The nanoplatform exhibits high stability and dispersity under physiological conditions. After intravenous injection, the nanoplatform could be precisely tracked in vivo and enabled laryngopharyngeal superficial cancer to be located and imaged. Combined photothermal therapy effectively ablated tumors with negligible side effects. Thus, this work presents a unique and biocompatible nanoplatform that allows multimodal imaging, high anti-tumor PTT efficacy, and negligible side effects in the treatment of laryngeal cancer.