Recent advances in the field of nanotechnology applications in nuclear medicine offer the promise of better diagnostic and therapeutic options. In recent years, increasing efforts have been focused on developing nanoconstructs that can be used as core platforms for attaching medical radionuclides with different strategies for the purposes of molecular imaging and targeted drug delivery. This review article presents an introduction to some commonly used nanomaterials with zero-dimensional, one-dimensional, two-dimensional, and three-dimensional structures, describes the various methods applied to radiolabeling of nanomaterials, and provides illustrative examples of application of the nanoscale radionuclides or radiolabeled nanocarriers in nuclear nanomedicine. Especially, the passive and active nanotargeting delivery of radionuclides with illustrating examples for tumor imaging and therapy was reviewed and summarized. The accurate and early diagnosis of cancer can lead to increased survival rates for different types of this disease. Although, the conventional single-modality diagnostic methods such as positron emission tomography/single photon emission computed tomography or MRI used for such purposes are powerful means; most of these are limited by sensitivity or resolution. By integrating complementary signal reporters into a single nanoparticulate contrast agent, multimodal molecular imaging can be performed as scalable images with high sensitivity, resolution, and specificity. The advent of radiolabeled nanocarriers or radioisotope-loaded nanomaterials with magnetic, plasmonic, or fluorescent properties has stimulated growing interest in the developing multimodality imaging probes. These new developments in nuclear nanomedicine are expected to introduce a paradigm shift in multimodal molecular imaging and thereby opening up an era of new diagnostic medical imaging agents. © 2018 Wiley Periodicals, Inc. J Biomed Mater Res Part A: 107A: 251-285, 2019.