Methyl jasmonate hormone can stimulate the production of several metabolites responsible for improving fruit quality and nutritional attributes related to human health. In this context, efforts to manipulate tomatoes, such as using hormonal treatment to increase metabolite levels essential to plant growth and human nutrition, have received considerable attention. The aim of this study was to show the impact of metabolic profile on fruit quality and nutritional properties under exogenous methyl jasmonate during fruit ripening. The treatments were performed using 100 ppm of methyl jasmonate and 100 ppm of gaseous ethylene over 24 h. Ethylene emission, fruit surface color and metabolomics analysis were measured at 4, 10, and 21 days after harvest, considering the untreated fruits as control group. Methyl jasmonate induced the production of amino acids—mainly glutamine, glutamic acid and γ-aminobutyric acid (at least 14-fold higher)—and fatty acids—mainly oleic, linoleic, and linolenic acids (at least three-fold higher than untreated fruits); while exogenous ethylene predominantly affected sugar metabolism, increasing the levels of fructose, mannose and glucose to at least two-fold that levels in the untreated fruits. Additionally, methyl jasmonate significantly affected secondary metabolites, inducing by at least 80% the accumulation of α-tocopherol and β-sitosterol in fully ripe fruits. Our results suggest that the postharvest application of the hormone methyl jasmonate can contribute to the sensory characteristics and increase the nutritional value of the fruits since important changes related to the tomato metabolome were associated with compounds responsible for the fruit quality and health benefits.