Exploring advanced co‐reaction accelerators with superior oxygen reduction activity that generate rich reactive oxygen species (ROS) has attracted great attention in boosting luminol‐O2 electrochemiluminescence (ECL). However, tuning accelerators for efficient and selective catalytic O2 activation to switch anodic/cathodic ECL is very challenging. Herein, we report that enzyme‐inspired Fe‐based single‐atom catalysts with axial N/C coordination structures (FeN5, FeN4(C) SACs) can generate specific ROS for cathodic/anodic ECL conversion. Mec...
