The advancement of novel materials to ameliorate interfacial charge transfer properties will drastically improve energy storage, heterogeneous catalysis, and various other electrochemical applications. Here we discuss a facile method that can utilize the Faradaic capabilities of residual iron nanoparticle catalysts that are captured within Multi-walled Carbon Nanotubes (MWNT) post-synthesis, thereby correcting the difficulties associated with creating hybrid nanocomposite electrodes. Non-purified MWNTs, experience a chemical oxidation procedure in an acidic environment with KMnO₄ to partly “unzip” the MWNTs and reveal the redox-active iron nanoparticles to the electrolyte. A consistent redox peak affiliated with the Fe^2+/3+ transition is achieved during the MWNT oxidation procedure yielding a ~350% improvement in capacitance (>300 F g^-1) when compared to purified MWNT electrodes (70 F g^-1). While these materials solely may be applicable as energy storage electrodes, the integration of redox species within an inert carbon electrode will also provide new opportunities to accelerate heterogeneous charge transfer reactions.