AbstractDisc membranes machined from high‐purity natural clinoptilolite rocks demonstrated promising hydrogen separation efficiency. However, these membranes cannot be adequately scaled up. To overcome this and provide process flexibility, mixed matrix membranes are required, pairing small particles of natural zeolite with a binder system. A novel approach was determined to use metals as binders and was tested by comparing natural clinoptilolite compact disc membranes with and without powdered copper metal. The phase composition and morphology of the discs were characterized and gas separation performance was evaluated using single gas permeation tests. Membrane selectivity for hydrogen separation was improved by applying metallic copper and copper oxide, filling a portion of the inter‐particle spaces and creating adhesion with the zeolite particles.