Physiological and metabolic profiles in tamarillo were investigated to reveal the molecular changes during fruit maturation. The firmness, ethylene production, soluble sugar contents, and metabolomic analysis were determined in tamarillo fruit at different maturity stages. The firmness of tamarillo fruit gradually decreased during fruit ripening with increasing fructose and glucose accumulation. The rapid increase in ethylene production was found in mature fruit. Based on the untargeted metabolomic analysis, we found that amino acids, phospholipids, monosaccharides, and vitamin-related metabolites were identified as being changed during ripening. The contents of malic acid and citric acid were significantly decreased in mature fruits. Metabolites involved in phenylpropanoid biosynthesis, phenylalanine metabolism, caffeine metabolism, monoterpenoid biosynthesis, and thiamine metabolism pathways showed high abundance in mature fruits. However, we also found that most of the mature-enhanced metabolites showed reduced abundance in over-mature fruits. These results reveal the molecular profiles during tamarillo fruit maturing and suggest tamarillos have potential benefits with high nutrition and health function.