Pentadesma butyracea is a medicinal plant of which bark decoctions are used in traditional medicine for the treatment of diarrhea symptoms in Gabon. The aim of the present work was to perform phytochemical and pharmacological analyses of decoctions of P. butyracea bark. In a principal approach, spectrophotometric analyses were used to quantify phenolic compounds, followed by liquid chromatography coupled to mass spectrometry analysis that allowed the identification of flavanone–flavone dimers as the main metabolites. Pharmacological analyses showed the absence of toxicity, thus confirming the safety of use of this decoction in traditional medicine. The antioxidant activity of the bark decoctions was demonstrated to depend on their phenolic contents. The decoction of stem barks harvested during the rainy season also induced a dose-dependent relaxation of isolated ileum fragments from Wistar rats. In addition, the antidiarrheal activity of P. butyracea barks was investigated against castor oil-induced diarrhea. The oral administration of different concentrations of this decoction led to a decrease in wet stools, indicating an antidiarrheal effect at the doses that were used. These results encourage the deepening of bio-guided research on P. butyracea bark decoctions in order to propose standard traditional medical treatments.