Calendering is a critical step in electrode manufacturing, as it determines electrode density and microstructure through mechanical compression. But calendered electrodes undergo time-dependent thickness recovery and microstructure evolution during storage, thereby increasing electrochemical resistance. This time-dependent spring-back is an overlooked yet critical factor governing the structural stability of calendered electrodes. Notably, this phenomenon is particularly pronounced in single-crystal cathodes, because their high mechanical robustness constrains the dissipation of compressive energy within particles during calendering. Here, we reveal that time-dependent spring-back is governed by the viscoelasticity of the carbon binder domain (CBD), which is inherently temperature-dependent. Specifically, polymer chain mobility within the CBD is enhanced at elevated temperature, which leads to change viscoelastic behavior of CBD toward a more viscous state. This enhanced fluid-like behavior allows the CBD to be more compliant under mechanical compression and effectively dissipate the applied stress, rather than storing it elastically. In a high-nickel single-crystal cathode active material (CAM), LiNi0.865Co0.054Mn0.075Al0.007O2, elevated-temperature (80°C) calendering effectively suppresses thickness recovery and microstructural relaxation during long-term storage. This suppression alleviates resistance growth and preserves electrochemical performance after prolonged storage. SEM image-based microstructure-resolved analysis further reveals that suppressed spring-back maintains higher CAM–CBD interfacial contact and a more homogeneous pore network within the electrode. Overall, this work establishes viscoelasticity of carbon binder domain as a key design parameter governing time-dependent spring-back in single-crystal cathodes, while highlighting temperature-controlled calendering as an effective strategy to ensure the long-term structural integrity.