Controllable preparation of water-soluble multifunctional nanoprobes is of great significance for cancer early diagnosis. In this study, protein-modified hydrophilic copper sufide (CuS) nanotriangles with tunable absorption in the second near-infrared region are developed in the presence of halide ions. Further, DTPA-Gd3+ is conjugated on it by using the unique characteristics of the protein-protected nanotriangles. Specifically, the as-obtained nanostructures are investigated as contrast agents for enhanced in vivo photoacoustic/magnetic resonance dual-modal tumor imaging. More importantly, in vitro and in vivo toxicity analysis are also performed, which show that the dual-modal nanoprobes are biocompatible for most of the cases. It is demonstrated that the novel as-prepared protein-modified nanotriangles are able to work as a nanoplatform to construct dual-modal nanoprobes, which paves a new anenue for improving the photoacoustic/magnetic resonance imaging contrast in cancer detection. Interestingly, other functional blocks may also linked on it, which makes it a general method to design multifunctional nanoprobes.