Blast-furnace slag (BFS) has been used as a feedstock for CO 2 sequestration by indirect mineral carbonation to produce calcium carbonate precipitates and solid residues. The most-abundant elements in these residues, Si and Al, are usually considered to be impurities that need to be removed in acid-dissolution processes involving BFS. The co-production of value-added materials from these residues is an attractive option for strengthening the economic competitiveness of mineral carbonation methods. In view of this, we separated the Si and Al, as their hydrated forms, during the dissolution of BFS in acetic acid prior to carbonation. During the sol-gel processing of Si-Al nanoparticles, a catalyst is usually required during the hydrolysis and subsequent condensation processes. In this study, only condensation occurs because the low-concentrations of acetic acid used facilitate in-situ hydrolysis during the dissolution process. Aging was carried out not only to structurally arrange the Si and Al but also to oxidize the marginal Fe(II) to reddish Fe(III). Silica-alumina nanoparticles (78% Si and 22% Al) were prepared by a simple sol-gel route at ambient pressure. These nanoparticles were amorphous and below 20 nm in size. Fourier-transform infrared (FT-IR) studies reveal that the nanoparticles consist of Si-O-Si and Si-O-Al bonds. 27 Al nuclear magnetic resonance (NMR) spectroscopy reveals a significant resonance corresponding to tetra-coordinated Al inside the particle framework.