Here, we adapt the catalytically self-threading polyrotaxane synthesis for the construction of two-dimensional polymeric thin films using a water−oil interfacial polymerization method. In this method, the polymerization and the rotaxane formation take place simultaneously at the interface because of the presence of catalytically active cucurbit[6]uril (CB6) that can facilitate 1,3-dipolar cycloaddition reaction between alkyne and azide to form polytriazoles. By varying the concentration of the

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... onomers, reaction time, and the size of the reaction vessel, it is possible to control the thickness and the lateral dimensions of the film. The as-synthesized film is free-floating, transparent, and robust enough to be transferred to any substrates. It contains photoactive porphyrin units which are quite appealing as a photosensitizer because of their capability to produce reactive oxygen species in high yield upon visible light irradiation. By taking advantage of these aforementioned features, this film was employed as a broad-spectrum photo-antimicrobial agent whose activity was switched on by light excitation against both Gram-negative and Gram-positive bacterial strains and switched off in the dark.