<p>The ever-growing population, changing climate, and the emergence of resistant variants of plant disease-causing pathogens have necessitated the need for new, improved, safe, and sustainable solutions to enhance the yield, curb the loss of crops to pests and diseases, and lengthen the shelf-life of the harvest to meet the increasing demand. In this current scenario, nanomaterials have emerged as a novel tool for resolving existing issues and incrementing crop yield and productivity. However, the limited knowledge about the uptake, mobilization, bioaccumulation, interactions, phytotoxicity, and biomagnification of nanomaterials in plants raises serious concerns regarding the safety of using nanomaterials in agriculture. The nanoparticle’s internalization, interactions, and effects on plants depend on their physicochemical characteristics, dose, and application routes. Different studies have reported nanomaterials’ positive and negative impacts on the plant system and agriculture. Nanomaterials have enhanced crop productivity by improving the germination rate of photosynthetic content, promoting growth and development, and providing resistance against stress, pests, and diseases. On the contrary, nanomaterials have also induced reverse phytotoxic effects by inhibiting germination, reducing plant growth, disrupting cellular metabolism by generating oxidative stress, and damaging proteins and DNA, thereby declining their yield. Considering this, the present review aims to outline the role of nanomaterials in enhancing crop productivity and their process of entry and translocation within plant systems while focusing on the different nanomaterial-induced implications in plants. It also discusses the different stress tolerance responses induced by the nanoparticles and molecular analysis of nanoparticle-induced phytotoxicity.</p>