Plastic and water pollution are two major environmental issues concerning human society since these pollutions continuously degrade the natural ecosystem and endanger living species. Polyethylene terephthalate (PET), one of the most commonly used plastics, accounts for a large portion of global plastic pollution. The recycling of PET wastes has great significance for human society and the natural ecosystem. However, current recycling methods suffer from lower economic and environmental benefits, which impedes their large-scale expansion. This work is designed to upcycle the PET-based wastes from everyday consumption sources (PET bottles and polyester fabric) into high added-value metal-organic framework materials (MOF) by reacting them with metal ions in the pickling wastewater via one-pot solvothermal synthesis method. Subsequently, the obtained MOF materials are used to purify water by adsorbing organic dyes. The study further analyzed the structural and adsorption properties of the obtained MOF. The results confirmed that the MOF materials, i.e., MIL-101, are synthesized successfully with a specific surface area of 2400-2600 m2 /g, which renders MIL-101 an excellent ability to remove dyes (i.e., rhodamine B (RHB) and methyl orange (MO)) from water, with adsorption efficiencies close to 100%. After the desorption tests, the MIL-101 materials were proved to be structurally intact, indicating their ability to go through multiple adsorption-desorption cycles. This work’s proposed strategy can lead to positive outcomes in the field of PET-based waste upcycling and water purification. This work opens a new avenue to treat pollution in a smart and efficient way and guide towards sustainable development.