Poly(vinyl alcohol) (PVOH)-based aerogel composites with nanoscale silica, halloysite, montmorillonite (MMT), and laponite were prepared via a freeze-drying method. The PVOH/MMT and PVOH/laponite composites exhibit higher compressive moduli than the PVOH/SiO2 or PVOH/halloysite samples. Layered microstructures were observed for the samples except with PVOH/laponite, which showed irregular network morphologies. Thermogravimetric analysis of the aerogel samples showed increased thermal stability with the addition of nanofillers. The heat release measured by cone calorimetry, smoke release, and carbon monoxide production of the aerogel composites are all significantly decreased with the addition of nanofillers; these values are much lower than those for commercial expanded polystyrene foam. The fillers did not lead to obvious increases in the limiting oxygen index values, and the corresponding time to ignition values decrease. The ability to adjust the nanofiller levels in these foamlike aerogel composites allows for specific tuning of these products for fire safety.