Herein, we report the in‐situ synthesis of amorphous GeSe/CNT composite via defective‐carbon‐mediated chemical bonding for ultrastable Na‐ion storage. Structural defects in CNTs play a crucial role in the chemical bonding and bonding strength in GeSe/CNTs composites. Specifically, the bonding strength tends to increase with increasing defect concentrations of CNTs. Remarkably, the strong chemical bonding between GeSe and CNTs significantly weakens Ge−Se bonds and promotes amorphization of GeSe, thus facilitating a reversible conversion reaction and enhancing Na‐ion diffusion. Consequently, GeSe/CNTs composite exhibits outstanding cyclability of 87.9% even after 1000 cycles at 1 A g−1 and a high‐rate capability of 288.3 mA h g−1 at 10 A g−1. Our work presents a promising approach for the amorphization of electrode materials enabled by the defective‐carbon‐mediated strong chemical bonding for Li‐, Na‐, and K‐ion batteries.