This study introduces a novel self-adaptive hierarchical carbon nanotube (CNT)-based host functionalized with cetyltrimethylammonium cations (CTA⁺) to address the challenge of dendrite formation in zinc-ion batteries (ZIBs). The CNT scaffold provides high flexibility and conductivity, enabling uniform Zn plating, while entangled CTA⁺ cations form switchable repulsive shields that dynamically suppress dendrite growth. Density functional theory (DFT) calculations confirm the effectiveness of the cationic shielding mechanism. The self-adaptive C-CNT host enables Zn symmetric cells to achieve an impressive cycling life of over 6500 hours at 1 mA·cm⁻² and a cumulative capacity of 6000 mAh·cm⁻² at 4 mA·cm⁻². Full batteries using C-CNT@Zn anodes and MnO₂ cathodes demonstrate 88% capacity retention after 2000 cycles at 2 A·g⁻¹. The design of the C-CNT host offers a promising approach for electrode-electrolyte interphase engineering in Zn-based energy storage systems. The C-CNT host effectively suppresses dendritic growth through dynamic regulation of Zn plating/stripping, enhancing the stability and reversibility of ZIBs. The study highlights the potential of the self-adaptive C-CNT host in enabling dendrite-free, high-performance ZIBs for practical applications.This study introduces a novel self-adaptive hierarchical carbon nanotube (CNT)-based host functionalized with cetyltrimethylammonium cations (CTA⁺) to address the challenge of dendrite formation in zinc-ion batteries (ZIBs). The CNT scaffold provides high flexibility and conductivity, enabling uniform Zn plating, while entangled CTA⁺ cations form switchable repulsive shields that dynamically suppress dendrite growth. Density functional theory (DFT) calculations confirm the effectiveness of the cationic shielding mechanism. The self-adaptive C-CNT host enables Zn symmetric cells to achieve an impressive cycling life of over 6500 hours at 1 mA·cm⁻² and a cumulative capacity of 6000 mAh·cm⁻² at 4 mA·cm⁻². Full batteries using C-CNT@Zn anodes and MnO₂ cathodes demonstrate 88% capacity retention after 2000 cycles at 2 A·g⁻¹. The design of the C-CNT host offers a promising approach for electrode-electrolyte interphase engineering in Zn-based energy storage systems. The C-CNT host effectively suppresses dendritic growth through dynamic regulation of Zn plating/stripping, enhancing the stability and reversibility of ZIBs. The study highlights the potential of the self-adaptive C-CNT host in enabling dendrite-free, high-performance ZIBs for practical applications.