Carbon nanotubes (CNT) are a family of carbon nanomaterials that have uses in many technological and medical applications due to their unique properties. However, compared to other nanomaterials, CNT have a significantly lower specific surface areas (SSA), which is a critical limitation for applications. To overcome this limitation, here, we report a new protocol to synthesize a hybrid material composed of varying ratios of multiwalled carbon nanotubes (MWCNT) and ferrihydrite (FHY). Furthermore, through a series of physical and electrochemical characterization tests, we determined that 36% FHY and 64% MWCNT is the optimum ratio for a composite that maximizes both SSA and specific capacitance. The calculated SSA of the composite was 190 m2·g−1, 2.9 times higher than that of MWCNT alone. Moreover, the composite retained valuable electrochemical properties of CNT with an estimated specific capacitance of 100 F·g−1. This composite is a promising multifunctional nanomaterial for environmental and technological applications requiring electrochemical reactivity and high specific areas such as environmental biosensors, and capacitive deionization for wastewater remediation, and water softening.