Traditional oil-in-water or water-in-oil emulsion has facilitated fabrication of materials. Here, we present the fabrication of living tissue-like materials that are made from a recently discovered water-in-water (w/w) emulsion. This w/w emulsion is comprised of dispersed droplets of liquid crystals formed by a non-amphiphilic molecule, disodium cromolyn glycate (DSCG) solvated in water. These water-based droplets are stabilized by polymer coatings that are also solvated in water. The stability of this novel system is primarily achieved by the separation of molecular interactions similar to those responsible for DNA duplex formation, and by multivalent interactions that prevent Ostwald ripening of colloidal materials. Extended from these fundamental sciences, we have developed a one-pot synthesis to produce protein laden porous hydrogel by cross-linking the carrier phase of this water-in-water emulsion; the protein monomers partition and concentrate in the interface of the droplet and the polymer coating. The activity of the immobilized proteins is highly retained and potentially enhanced for a wide range of enzymes, including horseradish peroxidase, amylase and aldolase. The structural characterization, including the spatial location of the enzymes in the hydrogel, and the quantification of the biocatalysis of the immobilized enzymes will be presented. Two mechanisms for potentially enhancing the enzymatic activity by this protein-laden hydrogel over enzymes in solution will be discussed. The use of this material for controlling biofilm formation on a wide range of surfaces and for developing sensors will also be presented.