A method for forming a super-insulating material for a vacuum insulated structure for an appliance includes disposing hollow glass spheres within a rotating drum, wherein a plurality of interstitial spaces are defined between the hollow glass spheres. An anchor material is disposed within the rotating drum. The hollow glass spheres and the anchor material are rotated within the rotating drum, wherein the anchor material is mixed with the hollow glass spheres to partially occupy the interstitial spaces. A silica-based material is disposed within the rotating drum. The silica-based material is mixed with the anchor material and the hollow glass spheres to define a super-insulating material, wherein the silica-based material attaches to the anchor material and is entrapped within the interstitial spaces. The silica-based material and the anchor material occupy substantially all of an interstitial volume defined by the interstitial spaces.