Globally, despite the commercial and cultural importance of edible caterpillars (Gynanisa maja and Gonimbrasia belina), comprehensive information on their dietary and therapeutic benefits has not been fully explored. The study was aimed at evaluating the nutritional composition and bioactive compounds profile of two important edible caterpillars (Gonimbrasia belina and Gynanisa maja) in Africa. Our results demonstrated that G. belina and G. maja are capable of amplifying host plant protein (17 %) by 4.3-folds [72.8 %] and 3.6-folds [61.3 %], respectively. Lysine (32.6 mg/g), methionine (12.5–27.1 mg/g) and valine (7.7–25.4 mg/g) value were significantly harnessed. Substantial amounts of ω−3 fatty acids (methyl 5Z,8Z,11Z,14Z,17Z-eicosapentaenoate and methyl 9Z,12Z,15Z-octadecatrienoate), minerals [iron (3.6–21.2 mg/100 g), zinc (7.1–17.3 mg/100 g), calcium (55.1–60.4 mg/100 g)] and vitamins [retinol (0.02–0.03 mg/kg), γ tocopherol (0.05–0.07 mg/kg) and α-tocopherol (1.2 mg/kg)] were detected. Important phytochemical [flavonoids: rutin (7.8–20.4 ng/g), quercetin (7.2–9.0 ng/g), luteolin (7.4–7.5 ng/g), apigenin (20.8–28.6 ng/g) and kaempferol (3.3–6.5 ng/g)] and phytosterols [stigmasta-3,5-diene, campesterol and sitosterol] were identified. These findings suggests that both edible caterpillars contain sufficient nutrients and therapeutic compounds, which when integrated into human food products, either whole, in-part, or processed will greatly contribute towards countering nutritional insecurity and improve livelihoods of people in many countries.