In this study, nitrogen‐doped carbon dots (N‐C‐dots) are synthesized via a green and gentle electrochemical‐hydrothermal method. The N‐C‐dots are grafted into the backbone of waterborne polyurethane (WBPU) synthesized from hexamethylene diisocyanate and polycarbonate diol (PCDL). Due to the introduction of N‐C‐dots, the WBPU is functionalized including being able to self heal and specifically identified Fe3+. The self‐healing performance of the WBPU‐N‐C‐dots film is principally attributed to the hydrogen bonding effect of the WBPU and the N‐C‐dots. On the other hand, based on the quenching of fluorescent characteristics of the WBPU‐N‐C‐dots film, it is successfully used in the detection of Fe3+, showing a wide detection range, good selectivity, and high sensitivity. What's more, the tensile strength of the sample is enhanced from 3.50 to 7.12 MPa when the N‐C‐dots content is increased in the WBPU and the thermal stability is improved as a result of the formation of the more thermally‐stable network structures. Interestingly, compared to the traditional solution detection in WBPU‐N‐C‐dots emulsion with the limit of detection of 2.23 × 10−6 m, the detection has the lower limit of detection of 2.19 × 10−6 m in the WBPU‐N‐C‐dots film. These results show that the WBPU‐N‐C‐dots film exhibits great application as an intelligent response‐type material.
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