The development of functional biomedicine for image-guided therapy has revolutionized the treatment of solid tumors, offering a precise, noninvasive approach to both diagnosis and therapy. Innovations in the design and development of biomedicines for image-guided surgery (IGS) have transformed the treatment of solid tumors. These image-guided surgeries feature precision and enhanced margins of safety for delicate cancerous tissues. This book chapter explores functional nanomaterials combined with imaging agents such as IRDye, lanthanides, actinides, and other metals. These functional biomedicines integrate with sophisticated imaging techniques, including computed tomography (CT), positron emission tomography (PET), cystoscopy, and magnetic resonance imaging (MRI), to improve patient treatment outcomes. The functional nanomedicines discussed include inorganic metallic and silica nanomaterials, carbon-based nanotubes, and fullerenes, alongside widely studied organic nanocarriers such as liposomes and polymeric carriers. These materials aim to enhance pharmacokinetics and pharmacodynamics (PK/PD), ultimately ensuring safety and efficacy. This class of nanomaterials offers unique benefits for image-guided surgery, with some still in the early stages of preclinical and clinical studies. Organic and polymer chemists have made significant advancements in nanomaterial design, biocompatibility, and safety. However, clinical translation and regulatory approval have faced considerable challenges, showing limited success. This chapter also discusses the opportunities and challenges for future research and development in functional biomedicine for image-guided surgery in solid tumors.