Membrane technology has been increasingly applied in water purification to address global water scarcity. However, commercial membranes inevitably reach the end-of-life (EoL) after long-term operation, which constrains the sustainability of membrane technology. Herein, we demonstrated the feasibility of upcycling real EoL poly(vinylidene fluoride) (PVDF) microfiltration (MF) membranes into reverse osmosis (RO) membranes with higher separation precision via the interfacial polymerization (IP) reaction. We highlighted that the EoL MF membrane, with a fouling-induced narrowed pore size and relatively hydrophobic properties, is preferred for upcycling. The resultant upcycled RO membrane exhibited a satisfactory NaCl rejection (98.6 ± 0.4%) with favorable water permeance (2.3 ± 0.7 L m