In this study, the challenge of non‐electrochemical activity in carbon nanotube fibers (CNTFs) is addressed by developing a modified chlorosulfonic acid (CSA) densification process specifically developed for directly spun CNTFs. This post‐treatment method, well‐known for enhancing the physical properties of CNTFs, utilizes the double diffusion phenomenon to efficiently integrate a diverse range of active materials, from conductive polymers like polyaniline (PANI) to metal oxides like nickel oxide (NiO), into the fibers. This universal and cost‐effective approach not only simplifies the integration process but also significantly boosts both the electrochemical and physical properties of the fibers. For instance, the PANI@CNTF composite exhibited a remarkable 17‐fold increase in specific capacitance and a two‐fold increase in load value compared to its pristine counterparts. This method proves straightforward, efficient, and versatile, making it suitable for developing fiber‐shaped electrodes that advance the capabilities of wearable energy storage systems.