Molecular imaging has significantly advanced the detection and analysis of in vivo metabolic processes, while single-modal techniques remain limited. Dual-modal imaging, particularly positron emission tomography (PET)-based combinations has emerged as a powerful solution, offering enhanced capabilities through integration with magnetic resonance imaging (MRI) or near-infrared fluorescence (NIRF) imaging. This review highlights recent progress in PET-based dual-modal imaging, focusing on the development of various bimodal probes derived from antibodies, nanoparticles, and peptides, and key applications including image-guided surgery and disease assessment. PET-based dual-modal imaging holds substantial potential for advancing research and diagnostics by improving resolution and providing functional insights. By combining complementary modalities, these systems deliver a more comprehensive view of disease processes, leading to more accurate diagnoses and targeted treatments. Future research prioritizes optimizing probe design for enhanced biocompatibility and safety, facilitating clinical translation, and broadens applications beyond cancer. Through interdisciplinary collaboration, PET-based dual-modal probes are poised to play a pivotal role in improving patient outcomes, particularly in diagnosing and managing complex diseases.