Nanomaterials (NMs) have shown relevant impacts in crop protection, improvement of yields, and minimizing collateral side effects of fertilizer and pesticides in vegetable and fruit production. The application of NMs to improve biofortification has gained much attention in the last five years, offering a hopeful and optimistic outlook. Thus, we propose comprehensively revising the scientific literature about the use of NMs in the agronomic biofortification of crops and analyzing the beneficial impact of the use of NMs. The results indicated that different species of plants were biofortified with essential elements and macronutrients after the applications of Zn, Fe, Se, nanocomposites, and metalloid NPs. In addition, the physiological performances, antioxidant compounds, and yields were improved with NMs. Using nanofertilizers for the biofortification of crops can be considered a promising method to deliver micronutrients for plants with beneficial impacts on human health, the environment, and agriculture.