Biological ion channels, as fundamental units participating in various daily behaviors with incredible mass transportation and signal transmission, triggered booming researches on manufacturing their artificial prototypes. Biomimetic ion channel with the nanometer scale for smart responding functions has been successfully realized in sorts of materials by employing state-of-art nanotechnology. Ion track-etching technology, as crucial branches of fabricating solid-state nanochannels, exhibits outstanding advantages, such as easy fabrication, low cost, and high customization. To endow the nanochannel with smart responsibility, various modification methods are developed, including chemical grafting, non-covalent adsorption, and electrochemical deposition, enriching the reservoir of accessible stimuli-responses combinations, whereas were limited by their relatively lengthy and complex procedure. Here, based on the electric field induced self-assembly of polyelectrolytes, a universal customizable modifying strategy has been proposed, which exhibits superiorities in their functionalization with convenience and compatibility. By using this protocol, the channels’ ionic transport behaviors could be easily tuned, and even the specific ionic or molecular responding could be realized with superior performance. This strategy surely accelerates the nanochannels functionalization into fast preparing, high efficiency, and large-scale application scenarios.