Abstract Integrated multimodal imaging in theranostics nanomaterials offers extensive prospects for precise and noninvasive cancer treatment. Precisely controlling the structural evolution of plasmonic nanoparticles is crucial in the development of photothermal agents. However, previous successes have been limited to static assemblies and single‐component structures. Here, an activatable plasmonic theranostics system utilizing self‐assembled 1D silver‐coated gold nanochains (1D nanochains) is presented for precise tumor diagnosis and effective treatment. The absorbance of the adaptable core–shell chain structure can shift from visible to near‐infrared (NIR) regions due to the fusion between nearby Au@Ag nanoparticles induced by elevated H 2 O 2 levels in the tumor microenvironment (TME), resulting in the creation of a novel 3D aggregates with strong NIR absorption. With a high photothermal conversion efficiency of 60.2% at 808 nm, nanochains utilizing the TME‐activated characteristics show remarkable qualities for photoacoustic imaging and significantly limit tumor growth in vivo. This study may pave the way for precise tumor diagnosis and treatment through customizable, optically tunable adaptive plasmonic nanostructures.