Mentha x piperitais a major source of secondary metabolites (SMs), and developing tools to enhance these compounds would be beneficial to meet the increasing demand in the industry. Elicitation by plant hormones became a new strategy to reach this goal. Three experiments in a climatic chamber and two experiments in an open field were conducted with peppermint to explore the effect of methyl jasmonate (MeJa) on the essential oil (EO) content, EO composition, and the total phenolic content (TPC). The treatment was applied for all experiments by spraying the aerial parts of the plants with a dosage of 2 mM MeJa twice. The treatment influenced all the parameters studied in the trials. The volatile content increased by 9–35%; however, in one trial it remained unchanged. The treatment also affected the main compounds of the EO. Menthone increased significantly in two trials while pulegone and menthofuran decreased. In the case of menthol, the change may also be influenced by the phenological and developmental stages of the plants. In the majority of cases, the TPC was also elevated considerably due to the treatments. MeJa treatments may have promising effects in influencing the accumulation of biologically active compounds and the quality of the drug; therefore, further systematic studies are needed to optimize the technology in vivo.