Pycreus smithianustubers have been reported to have insecticidal properties. To gain further insight into its medicinal values, phytochemical and antimicrobial studies were carried out on its shoot and root. The phytochemical screening indicated the presence of reducing sugars, tannins, flavonoids, terpenoids, cardiac glycosides, and saponins in varying quantities as well as absence of steroids and alkaloids. Aqueous and ethanolic extracts (shoot and root) were tested against two fungi—Aspergillus nigerandCandida albicans—and two bacteria—Staphylococcus aureusandSalmonella typhi. Antimicrobial activity evaluation was carried out at 50 and 100 mg/mL concentrations by Agar Well Diffusion method. From the antimicrobial evaluation, the root ethanolic extract at 100% concentration was the most effective againstS. aureusandC. albicanswhile the shoot ethanolic extract was effective againstS. typhi. No extract was active againstA. niger. Ethanolic extracts were more active than the aqueous extracts and showed higher inhibitory activity against the bacteria than the fungi. This is most likely due to the abundance of reducing sugars in the ethanolic extracts. From these findings, ethanolic extracts of the root ofP. smithianusexhibited a good potential source of new drug for treating infections caused by these pathogens and particularly drug resistantC. albicans.