Abstract Surface antibacterial coatings with outstanding antibacterial efficiency have attracted increasing attention in medical protective clothing and cotton surgical clothing. Although nanozymes, as a new generation of antibiotics, are used to combat bacteria, their catalytic performance remains far from satisfactory as alternatives to natural enzymes. Single‐atom nanodots provide a solution to the low catalytic activity bottleneck of nanozymes. Here, atomically thin C 3 N 4 nanodots supported single Cu atom nanozymes (Cu‐CNNDs) are developed by a self‐tailoring approach, which exhibits catalytic efficiency of 8.09 × 10 5 M −1 s −1 , similar to that of natural enzyme. Experimental and theoretical calculations show that excellent peroxidase‐like activity stems from the size effect of carrier optimizing the coordination structure, leading to full exposure of Cu‐N 3 active site, which improves the ability of H 2 O 2 to generate hydroxyl radicals (•OH). Notably, Cu‐CNNDs exhibit over 99% superior antibacterial efficacy and are successfully grafted onto cotton fabrics. Thus, Cu‐CNNDs blaze an avenue for exquisite biomimetic nanozyme design and have great potential applications in antibacterial textiles.