Amyloid-like fibrils have a relatively high specific surface area, which makes them suitable as absorbents. In this study, we prepared absorbent composite aerogels from whey protein isolate fibril (WPIF) and calcium alginate (CA). The impact of protein fibrillation time (4-24 h) on the adsorption properties of these aerogels was assessed, as this influences the nature of the WPIFs formed. Fourier transform infrared spectroscopy analysis indicated that hydrogen bonding, hydrophobic interactions, and electrostatic interactions were the main molecular interactions in the composite aerogels. Then, the adsorption properties of the aerogels were investigated using crystal violet as a model compound. The adsorption properties of all composite aerogels were significantly improved compared to CA aerogels, which was mainly attributed to the numerous functional groups of the surfaces of the WPIFs, as well as the rougher surface topology of the composite aerogels. The adsorption capacity of the composite aerogels first increased and then decreased with increasing fibrillation time, with 8 h fibrillation leading to the largest adsorption capacity (1886.11 mg/g). Thioflavin T fluorescence, atomic force microscopy, light extinction, average particle size, and zeta potential analysis indicated that the high fibril content, mature fibril morphology, large number of available functional groups on the surface, and relatively low zeta potential of WPIF8 might be the main reasons. Adsorption kinetics and isothermal adsorption profile analysis suggested that monolayer adsorption occurred through chemical adsorption processes. The edible aerogel with high adsorption properties developed in this work has potential application in food and biomedical fields.