Introducing green technologies and minimising the use of synthetic and toxic compounds are the most important steps to overcome the environmental obstacles in textile finishing. Another essential requirement for a better life is the prevention of waste, which negatively impacts the environment, economy and human health. This chapter presents a comprehensive study on the development of a novel and environmentally friendly synthesis of zinc oxide (ZnO) using aqueous extracts from plant waste and gaseous plasma technology, directly (in situ) on cotton and polyethylene terephthalate (PET), to obtain fabrics with ultraviolet (UV)-protective and hydrophobic or hydrophilic properties. Plant waste from the food processing industry and invasive alien plants were used as a source of phytochemicals in in situ ZnO synthesis. ZnO is an inorganic compound that is widely used in various industries due to its multifunctional properties. It can exhibit UV-protective, antimicrobial, self-cleaning, hydrophobic and other properties when applied to textiles. The chapter investigates different methods and parameters to achieve the most optimised synthesis procedure to enable textiles with functional protective properties. It also discusses the importance of the selection of a plant-based reducing agent in ZnO synthesis, the use of gaseous plasma and its effect on polymer modification and assistance in ZnO synthesis.