(1) Plants, due to their phytochemicals, have long been known for their pharmacological potential and medicinal value. Verjuice, the acidic juice of unripe green grape, is still poorly characterized in terms of its chemical composition and biological activities. (2) In this study, we characterized the chemical composition, antioxidant and antitumor potential of verjuice extract. Folin–Ciocalteu and aluminum chloride reagents were used to identify the total phenol and total flavonoid composition. Various conventional methods were used to quantify the alkaloids and tannins. DPPH (2,2-diphenyl-1-picrylhydrazyl) free radical scavenging assay and Neutral Red assay were used to assess the antioxidant and antitumor activities, respectively. (3) We showed that the verjuice extract contains alkaloids, tannins, and a high quantity of total flavonoids and total phenols. Besides its antioxidant activity, verjuice significantly repressed human pulmonary adenocarcinoma (A549) cells’ viability in both dose- and time-dependent manners. Moreover, verjuice extract significantly enhanced the anticancer potential of cisplatin. (4) Altogether, these observations suggest a potential use of verjuice as a natural antitumor remedy.