AbstractThe preparation of resistant ultrathin film (utf) hydrogels coated onto different working surfaces (e.g., fabrics) is paying increasing attention as an advantageous strategy for customizing their resultant properties. More specifically, poly(ethylene glycol) (PEG)‐based utf‐hydrogels are relevant for their superior biocompatibility or antibiofouling properties. However, promoting the generation of poly(ethylene glycol) dimethacrylate (PEGDMA) cross‐links ideally without the use of initiators or other cross‐link agents, which might compromise the final bioactivity of the system, is complicated. Moreover, the actual synthesis techniques used for the preparation of such utf‐hydrogels face important drawbacks like high scale‐up costs or important geometrical restrictions, completely hindering its technological transfer. Herein, for the first time and easy and technologically scalable technology is reported for the synthesis and direct deposition of PEGDMA400 utf‐hydrogels onto different substrates based on atmospheric pressure nanosecond pulsed plasma approach. The advantages of the technology are explored and discussed, reporting the ready‐to‐use transparent coating of fabrics. After washing the samples using washing programs of a commercial laundry machine, coatings are still well adhered, showing excellent stability. Finally, the resultant properties of PEGDMA400 utf‐hydrogels are exhaustively characterized using in operando conditions in order to elucidate their potential capabilities in the biomedical field.