There is a growing interest in developing agricultural practices that can improve crop performance while preserving natural resources. Plant biostimulants are thought to play a role in reaching this goal, in particular by increasing the nitrogen use efficiency. However, a notable research gap exists concerning the effects of foliar applications of natural zeolites as plant biostimulants on crop performance. To address this knowledge gap, a greenhouse experiment was set up in order to study the response of maize and wheat traits, specifically the biomass productivity and nitrogen uptake, as well as the response of soil extracellular enzymes to the foliar applications of a natural zeolite in combination with different levels of nitrogen fertilization, that is, 100%, 75%, and 50% of the optimal dose. Foliar application of zeolite in wheat and maize plants led to an increase in root nitrogen concentration of about 10%, particularly at the lowest nitrogen fertilization rate. This response was accompanied by an increase in aboveground to belowground uptake nitrogen ratio. Furthermore, there was a significant reduction of about 20% in root biomass in both crops with zeolite application across the entire nitrogen fertilization gradient. These plant-level responses were associated with a significant increase in the activity of carbon-degrading and nitrogen-degrading enzymes at the soil level in response to zeolite applications. Our findings provide a compelling proof-of-concept for the beneficial effects of foliar-applied zeolite as a biostimulant for crops, emphasizing the critical need for additional field research to validate our greenhouse results.