Abstract: The present invention provides methods and devices for augmenting impaired glycocalyx barrier function in a subject in need thereof by contacting a sample (e.g., blood) obtained from the subject with a glycocalyx-mimetic adsorption media. The adsorption media includes glycosaminoglycan structures and, optionally, proteoglycan core proteins, which are conducive to enhancing and/or restoring the impaired glycocalyx barrier function in a sample. The contacted sample is subsequently separated from the adsorption media, producing a treated sample that can be infused into the subject. Methods and devices for treating a patient suffering from a disease associated with glycocalyx barrier dysfunction are also provided herein.