This study examined the qualitative and quantitative phytochemical composition of Datura stramonium (leaves, flowers, fruits, stems) and Garcinia kola (seed and seed coat) using successive solvent extractions and standard phytochemical screening methods. Qualitative phytochemical analysis revealed solvent-dependent variations. In D. stramonium, methanol and ethyl acetate extracts of leaves showed the presence of alkaloids, flavonoids, and saponins, while dichloromethane and n-hexane extract predominantly contained alkaloids and steroids. Flowers exhibited alkaloids in all extracts, flavonoids and saponins mainly in methanol and ethyl acetate, and steroids in nonpolar solvents. Fruits displayed alkaloids across all solvents, flavonoids chiefly in methanol, and steroids in dichloromethane and hexane. Stems showed alkaloids in methanol, ethyl acetate, and dichloromethane, with steroids and tannins restricted to dichloromethane and hexane. For G. kola, seeds contained alkaloids in methanol and dichloromethane, flavonoids in all solvents, saponins in methanol and dichloromethane, and steroids in ethyl acetate and hexane. The seed coat exhibited alkaloids only in methanol, flavonoids in methanol and dichloromethane, tannins in methanol and dichloromethane, and steroids in ethyl acetate and hexane. Quantitative analysis revealed that alkaloids were highest in D. stramonium leaves (10.60 ± 0.53%) and fruits (10.40 ± 0.23%) as well as in G. kola seeds (9.30 ± 0.86%). Flavonoids peaked in G. kola seeds (14.00 ± 0.23%) and D. stramonium flowers (7.20 ± 0.29%), while saponins were abundant in D. stramonium leaves (11.40 ± 0.25%) and G. kola seeds (11.50 ± 0.08%). Tannin levels were generally low (<1.30%), with the highest in G. kola seed coat (1.26 ± 0.21%). In conclusion, the phytochemical richness of D. stramonium and G. kola validates their traditional use and highlights their potential as valuable sources of bioactive compounds.