In this study, O-amino benzenethiol (OABT) was oxidized in one pot using Fe(NO3)3 to produce a novel Fe2S3-Fe2O3/poly O-amino benzenethiol (POABT), which showed a highly uniform morphology. At the same time, from SEM analysis, highly wrinkled porous polypyrrole (Ppy) and porous ball-like POABT structures prepared from the K2S2O8 route were evidenced by SEM and TEM analyses. A nanocomposite pseudo-supercapacitor (SC) was fabricated using Fe2S3-Fe2O3/POABT, and its performance was tested with and without incorporating Ppy in the paste. The results indicate that Ppy significantly increased the specific capacitance (CS) values, indicating an enhancement in charge storage. At a current density of 0.2 A/g, the CS values were 44 F/g and 161 F/g for the paste without and with Ppy, respectively. Additionally, the E was calculated, and the incorporation of Ppy resulted in a significant increase in E, reaching 30 W.h.kg−1; this was significantly higher than the value of 8.18 W.h.kg−1 observed without Ppy materials. This effect is likely due to the improved charge transfer facilitated by the presence of Ppy, as evidenced by the Nyquist plot, where the Rct values were 1.1 Ω and 2.1 Ω with and without Ppy, respectively. Overall, the low cost and significant technical advantages of this capacitor make it a promising candidate for commercial applications.