Pseudocapacitance has been confirmed to significantly improve the rate capability and cycling durability of electrode materials. However, rational design and controllable synthesis of intercalation pseudocapacitive materials for sodium-ion batteries (SIBs) still remain greatly challenging. Herein, a coreâshell TiO 2 -based anode composed of S-, Co-, and N-doped amorphous TiO 2 /C framework cores and ultrathin anatase TiO 2 nanosheet shells (SCN-TC@UT) was synthesized using Ti-based metalâorganic frameworks (Ti-MOFs) as self-sacrificing templates coupled with a solvothermal sulfidation process. Thanks to heteroatom doping, integration of carbon species, and 2D nanosheet coating, the kinetic properties of SCN-TC@UT have been significantly improved. As a consequence, the anode achieves ultrahigh capacitive contributions up to 90.9 and 96.3% of the total capacity at scan rates of 5 and 10 mV s â1 and delivers unprecedented capacities of 211, 201, and 100 mA h g â1 at 1, 5, and 30 C (1 C=335 mA g â1 ) for over 800, 2000, and 18,000 cycles, respectively. Even at an ultrahigh rate of 50 C, the anode can still deliver a capacity of 108 mA h g â1 . This work demonstrates the most efficient TiO 2 -based anode ever reported for SIBs and holds great potential in directing the development of amorphous materials for intercalation pseudocapacitance.