Over the past two decades, amorphous nanoscale coordination polymers (NCPs) and crystalline nanoscale metal-organic frameworks (NMOFs) have emerged as attractive nanomaterials in biomedical applications, especially in drug delivery, biomedical imaging, and biosensing. The biodegradability, tunable composition, and feasible functionality of NCPs/NMOFs make them excellent contrast agents or nanocarriers for biomedical imaging, including magnetic resonance (MR) imaging, positron emission tomography (PET), computed tomography (CT), optical imaging, and photoacoustic (PA) imaging. In this Topical Review, we will summarize the recent advances of NCPs/NMOFs in biomedical imaging with emphasis on research over the past three years. A variety of imaging technologies based on NCPs/NMOFs will be discussed, followed by the introduction of the application of NCPs/NMOFs in multimodal imaging where optical/MR imaging is highlighted. In the final part, we will make concluding remarks and point out the challenges and prospects for the further development in this area of research.