We report a novel and flexible surface enhanced Raman scattering (SERS) substrate based on filter membranes decorated with silver dendritic nanostructures. The SERS-active substrate was fabricated via electrodeposition, where hierarchical silver dendrites were uniformly and firmly deposited within and on the top of the porous filter membranes. The morphological evolution of silver dendrites was investigated at different deposition times, and the effect of the components of electrolyte was also studied. Finite difference time domain (FDTD) simulations were performed to reveal the distribution of electric filed when Ag dendrites were illuminated with 785 nm light. Such 3D SERS-active substrate exhibits extremely high sensitivity and excellent reproducibility. Raman signal sensitivity for rhodamine 6G was tested as high as 1 × 10^?11 M with 12% average intensity variations at the major Raman peak. Additionally, the as-synthesized robust substrate displays high stability under an ambient condition for several months. This 3D eco-friendly filter membrane-based substrate provides not only high density of SERS hot spots, but also a very large area for capturing target analytes. It has potential applications for the detection of trace organic contaminants in the environment.