The conductive skeleton and aligned carbon nanotube array (CNTA) structure can greatly shorten the ion transfer path and promote the charge transfer speed, which makes the CNTA an ideal electrode material for energy storage application. However, poor mechanical stability and low specific capacitance greatly impede its practical utilization. Here, we introduce a promising flexible electrode material based on the natural spider silk protein (SSP) modified CNTA(SSP/CNTA) with improved hydrophilicity and mechanical flexibility. The redox-active Fe
