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Abstract Ion‐insertion capacitors show promise to bridge the gap between supercapacitors of high power densities and batteries of high energy densities. While research efforts have primarily focused on Li⁺‐based capacitors (LICs), Na⁺‐based capacitors (SICs) are theoretically cheaper and more sustainable. Owing to the larger size of Na⁺compared to Li⁺, finding high‐rate anode materials for SICs has been challenging. Herein, an SIC anode architecture is reported consisting of TiO₂nanoparticles anchored on a sheared‐carbon nanotubes backbone (TiO₂/SCNT). The SCNT architecture provides advantages over other carbon architectures commonly used, such as reduced graphene oxide and CNT. In a half‐cell, the TiO₂/SCNT electrode shows a capacity of 267 mAh g⁻¹at a 1 C charge/discharge rate and a capacity of 136 mAh g⁻¹at 10 C while maintaining 87% of initial capacity over 1000 cycles. When combined with activated carbon (AC) in a full cell, an energy density and power density of 54.9 Wh kg⁻¹and 1410 W kg⁻¹, respectively, are achieved while retaining a 90% capacity retention over 5000 cycles. The favorable rate capability, energy and power density, and durability of the electrode is attributed to the enhanced electronic and Na⁺conductivity of the TiO₂/SCNT architecture.