Animal-based whey protein isolate (WPI) and plant-based potato protein isolate (PPI) aerogel microparticles (particle size ∼40–77 μm) were produced via top-down wet milling of alcogels followed by supercritical–CO2–drying and used as matrices for structuring of liquid sunflower oil. pH variation (pH 3.0, 7.0, 9.0) during heat-induced gelation was used to tune aerogel microstructural properties, resulting in high specific surface areas (347–480 m2/g) and mesopore volumes (2.3–5.6 m3/g) as well as different macro-to mesoporous ratios. Oleogels oil content (70–84 wt%) and firmness (0.55–1.25 N) were related to pH during gelation, yielding firmest oleogels for aerogel templates produced at pH 9. All oleogel samples showed high physical stability, as shown by oil holding capacity (OHC) up to 95%. Minimization of macropore volume, high mesopore fractions, and high specific surface areas were found to increase OHC. Results suggest that for WPI and PPI, different aerogels microstructures induced by different gelation pH rather than protein nature, to be the driving factor affecting aerogel oleogelation ability and demonstrate the versatility of the aerogel particle-template approach in terms of protein source, thus highlighting the importance of aerogel microstructure design to fine-tune oleogel properties.
