Today, demand exists for new systems that can meet the challenges of identifying biological entities rapidly and specifically in diagnostics, developing stable and multifunctional membranes, and engineering devices at the nanometer scale. In this respect, bio-decorated membranes combine the specificity and efficacy of biological entities, such as peptides, proteins, and DNA, with stability and the opportunity to chemically tailor the properties of polymeric membranes. A smart strategy that serves to fulfill biological criteria is required, whereby polymer membranes come to mimic biological membranes and do not disturb but rather enhance the functioning and activity of a biological entity. Different approaches have been developed, exemplified by either planar or vesicular membranes, allowing insertion inside the polymer membrane or anchoring via functionalization of the membrane surface. Inspired by nature, but incorporating the strength provided by chemical design, bio-decorated polymer membranes represent a novel concept with great potential in diagnostics and therapeutics.