World fiber production and demands are constantly increasing over the years, with textile wastes being a part of increasing environmental and economic problems. One of the biggest challenges with recycling textiles is the multitude of multi-material textiles, especially fabrics that consist of a blend of two or more different types of fibers. The use of multi-materials fiber in textiles and its recycling has been identified as a bottleneck in textile waste management and the challenge of fibre separation from blends needs to be solved. Acrylic fiber is one of the fibers commonly used in multi-material textiles because of its outstanding properties and performance. To overcome this hurdle, an effective technique has been demonstrated for the first time for acrylic fiber by enabling chemical upcycling technology for the separation of fibre blends containing synthetic and cellulosic fibers. This developed technology for upcycling acrylic textile blends enables both main products as polyacrylate solutions and acquiring recycled other blend textiles from their final thread, fabric, and cloth forms and regenerated synthetic and cellulosic. The selective and environmentally benign green method developed in this work demonstrates an example of a future sustainable textile application for the first time an effective recycling strategy for acrylic fabric blends. Acrylic fiber containing such fiber blends is part of the increasing environmental and economic problems associated with textile waste. Effective recycling of textiles through the separation of constituent fibers will drive the textile industry towards a circular economy model.