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Simple Summary: The development of novel cancer treatment techniques is essential because malignant tumors represent a severe threat to human life and health. By inhibiting immunological sites and chimeric antigen receptors, tumor immunotherapy is becoming more and more significant. There are several immune cells linked to tumors, and NK cells are one type that is being utilized more and more in therapeutic settings because of the inherent benefits. Additionally, the anti-tumor immune response and NK cell-tracking ability are improved by the use of nanomaterials. In order to accomplish the combined application of NK cells and nanomaterials, this review will concentrate on the immunological application and imaging study of nanoparticles on NK cells. The prognosis for cancer patients has declined dramatically in recent years due to the challenges in treating malignant tumors. Tumor immunotherapy, which includes immune target inhibition and chimeric antigen receptor cell treatment, is currently evolving quickly. Among them, natural killer (NK) cells are gradually becoming another preferred cell immunotherapy after T cell immunotherapy due to their unique killing effects in innate and adaptive immunity. NK cell therapy has shown encouraging outcomes in clinical studies; however, there are still some problems, including limited efficacy in solid tumors, inadequate NK cell penetration, and expensive treatment expenses. Noteworthy benefits of nanomaterials include their chemical specificity, biocompatibility, and ease of manufacturing; these make them promising instruments for enhancing NK cell anti-tumor immune responses. Nanomaterials can promote NK cell homing and infiltration, participate in NK cell modification and non-invasive cell tracking and imaging modes, and greatly increase the effectiveness of NK cell immunotherapy. The introduction of NK cell-based immunotherapy research and a more detailed discussion of nanomaterial research in NK cell-based immunotherapy and molecular imaging will be the main topics of this review. [ABSTRACT FROM AUTHOR]