Background: Solanum aculeastrum is reportedly used in several diseases including gonorrhea, bronchitis, jigger infestations and wounds, and cancers. We conducted an exhaustive phytochemical and GC-MS profiling of its methanol extract and solvents’ fractions. Methods: About 4500g of dried berries of S. aculeastrum was extracted with methanol, part of which was partitioned into fractions of n-hexane, dichloromethane, ethyl acetate, n-butanol and aqueous fractions. These fractional preparations were subjected to phytochemical and GC-MS profiling except aqueous fraction. Results: The percentage yield of 430.69g of methanol extract of berries of S.aculeastrum was 9.57%w/w, while the yields of dried 19.4g of n-hexane, 38.4g of DCM, 6.4g of ethyl acetate, 81.03g of n-butanol and 21.2g of the freeze-dried aqueous fractions were 7.08%w/w, 14.03 %w/w, 2.33%w/w, 29.60%w/w and 7.74%w/w respectively. The relative presence of glycosides, alkaloids, tannins, flavonoids, terpenoids, phenols, saponins were confirmed except quinones. GC-MS profiling of methanol extract identified 32 compounds including alkane, alcohol, carbohydrate, fatty acids, terpenoids, glycerides, vitamins and some unclassified compounds. 25 compounds including terpenoids, alkene, fatty acids, vitamin and unclassified compounds were identified in n-hexane fractions. The DCM fraction yielded 20 compounds including isoprenoid, terpenoids, amino acids, carboxylic acid and unclassified compounds. 22 compounds were identified in ethyl acetate fraction including phenol, fatty acids, alcohol, terpenoids, glycerolipid and unclassified compounds. The n-butanol fraction yielded 11 compounds including fluorinated aromatic substance, hormonal antineoplastic and a non-steroidal anti-inflammatory agent. Conclusion: This study has further elaborated on the bioactive compounds in berries of S. aculeastrum, to aid robust understanding of its pharmacologic activities.