Rezak et al reports the use of peptidic dynamic covalent polymers (DCPs) for stabilizing AuNCs, which can lead to enhanced NIR-II luminescence due to balanced ligand rigidification and hydrophobicity. The results are interesting, which suggest the potential use of DCPs for enhancing the optical property of metal NCs. The manuscript can be considered for publication after properly addressing my following corcerns.

The distinct advantage of DCPs in modulating the optical property of AuNCs has not been clearly demonstrated or discussed in the manuscript. The authors are suggested to strengthen this issue.

Nanoprobes with hydrophobic ligands on the surfaces may compromise their further use in biological imaging due to limited water-dispersity and stability in aqueous medium. Please consider this in the discussion or add relevant data.

The origin of their NIR-II luminescence should be discussed to better understand their optical properties and the enhancement mechanism (e.g., see ref Journal of Analysis and Testing 2023, 7, 260-271). Lifetime and XPS characterization are suggested to be considered.

Minor issues. Figure S10, the unit of x-axis should be Wavenumber instead of Wavelength.

The authors have well addressed my concerns. Publication is recommended.