This study presents an eco-friendly protocol for the hydrophilization of polyethylene terephthalate (PET) fabric and the in situ synthesis of ZnO particles. The alkaline medium and reducing agent for ZnO synthesis were prepared as aqueous extracts from wood ash and pomegranate peel, respectively. Due to the hydrophobic nature of the PET fabric, oxygen plasma treatment was included in the process. The influence of plasma treatment in different synthesis steps on the formation of ZnO and consequently on the morphological, colour and ultraviolet (UV) protective properties of the samples was discussed. The study showed that incorporating oxygen plasma treatment before immersing the samples in each solution for the ZnO in situ synthesis (natural alkaline medium of wood ash, zinc salt and natural reducing agent from pomegranate peel) produced PET fabric with the most uniform ZnO layer without visible cracks and the highest UV-blocking ability with a UV protection factor (UPF) of 300+. The colour measurements showed that increasing the number of plasma treatments leads to higher colour strength of the samples. Herein, a novel protocol for the production of protective PET fabrics is presented, which is also an example of a completely environmentally benign textile functionalization process.