The milk fat globule membrane, present in buttermilk, contains complex lipids such as phospholipids. Microfiltration coupled with supercritical fluid extraction (SFE) may provide a method of enriching these nutritionally valuable lipids into a novel ingredient. Therefore, SFE as a method for phospholipid enrichment needs to be optimized for lipid removal effectiveness. The role of matrix additions to the buttermilk powder for extraction efficiency was evaluated. Diatomaceous earth (biosilicates), Teflon beads, and physical vibration were tested and shown to reduce total lipid by 86, 78, and 70%, respectively. Four consecutive treatments were shown to exhaust the system; however, similar extraction efficiencies were noted for 1 treatment with biosilicate addition, 2 treatments with physical vibration, or 3 treatments with added Teflon beads. The extracted lipid material consisted of the nonpolar fraction, and protein concentration was observed to increase slightly compared with the control. Although higher lipid extraction was achieved from the powder with addition of diatomaceous earth, a removable aid is ideal for an edible product.