This study presents a novel triple-modality nanoparticle (MPR) for molecular imaging of brain tumors, combining Magnetic Resonance Imaging (MRI), Photoacoustic Imaging, and Surface Enhanced Raman Scattering (SERS). The MPRs, composed of a 60 nm gold core coated with a Raman molecular tag and a 30 nm silica shell, were designed to be retained by tumors due to the enhanced permeability and retention (EPR) effect. In vitro and in vivo experiments demonstrated that MPRs could be detected with picomolar sensitivity across all three modalities, allowing for accurate tumor delineation both pre- and intra-operatively. MRI provided whole-brain tumor localization, Photoacoustic imaging offered high spatial resolution, and Raman imaging enabled high sensitivity and specificity in detecting tumor margins. Histological validation confirmed the accurate delineation of tumor borders, and intra-operative Raman imaging guided precise tumor resection, revealing microscopic tumor extensions not visible by visual inspection alone. This approach holds promise for more accurate brain tumor imaging and resection.This study presents a novel triple-modality nanoparticle (MPR) for molecular imaging of brain tumors, combining Magnetic Resonance Imaging (MRI), Photoacoustic Imaging, and Surface Enhanced Raman Scattering (SERS). The MPRs, composed of a 60 nm gold core coated with a Raman molecular tag and a 30 nm silica shell, were designed to be retained by tumors due to the enhanced permeability and retention (EPR) effect. In vitro and in vivo experiments demonstrated that MPRs could be detected with picomolar sensitivity across all three modalities, allowing for accurate tumor delineation both pre- and intra-operatively. MRI provided whole-brain tumor localization, Photoacoustic imaging offered high spatial resolution, and Raman imaging enabled high sensitivity and specificity in detecting tumor margins. Histological validation confirmed the accurate delineation of tumor borders, and intra-operative Raman imaging guided precise tumor resection, revealing microscopic tumor extensions not visible by visual inspection alone. This approach holds promise for more accurate brain tumor imaging and resection.