Niobium-based Wadsley–Roth (ReO3-type shear) oxides are promising intercalation anodes for fast-charging and safe lithium-ion batteries owing to their open frameworks and relatively high operating potentials; however, their practical use is still hindered by limited electron/ion transport and insufficient reversible capacity. Herein, we synthesize In3+-doped In0.5Nb24.5O62 via a solvothermal–calcination route and demonstrate that In3+ doping triggers a defect-rich ReO3-type shear structure with expanded lattice parameters and abundant cation-vacancy/defect features. Such a structural modulation widens Li+ migration channels and creates additional electrochemically active sites, thereby accelerating charge transport and Li+ diffusion kinetics. Importantly, we systematically correlate calcination temperature and duration with phase evolution, defect/crystallite development, and rate/cycling behavior, identifying 1000°C for 6 h as an optimal condition that balances moderate crystallinity and high defect density for fast yet stable lithiation/delithiation. As a result, the optimized anode delivers a high initial charge capacity of 359.24 mAh g-1 at 0.1 C, retains 157.33 mAh g-1 at 20 C, and maintains 210.49 mAh g-1after 500 cycles at 10 C with a capacity retention of 97.5 %. Density functional theory further reveals that In3+ doping reduces the band gap and decreases Li adsorption/formation energies, while providing more favorable adsorption sites and additional diffusion pathways with reduced barriers, rationalizing the enhanced fast-charging performance. This work highlights a general strategy of dopant-induced defect shear engineering combined with precise thermal-treatment control for designing high-rate and long-life niobium-based intercalation anodes.
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