In this work, an aerogel with excellent flame retardancy, enhanced compression modulus, and efficient thermal insulation was developed from poly(vinyl alcohol) (PVA), biobased phytic acid (PA), and single-walled carbon nanohorns (SWCNHs). The microstructural evolution of the freeze-dried PVA/PA/SWCNH composite aerogels revealed that varied amounts of phytic acid could influence the three-dimensional architecture. Especially, when the concentration of PA was 1.5%, the PVA/PA/SWCNHs composite aerogel with a tightly arranged "short tubes" structure had a high compressive modulus of 2.02 MPa, corresponding to the specific modulus of 20.2 MPa cm 3 /g. Compared to the PVA/SWCNHs aerogel, the PVA/PA/SWCNHs composite aerogels showed better fire retardancy, as confirmed by limited oxygen index (LOI) tests and cone calorimetry (CC) tests. Notably, the introduction of phytic acid at 1.5% resulted in LOI values up to 49.8 ± 0.1% and the pHRR and THR of the PVA/PA/SWCNHs composite aerogel were dramatically reduced by 74.3 and 81.0%, respectively. In addition, PVA/PA/SWCNHs composite aerogels with different concentrations of phytic acid exhibited excellent thermal insulation performance with a slightly lower thermal conductivity (32.2− 46.9 mW/(m K)) and resisted the ∼1300 °C flame. Meanwhile, the synergistic flame retardancy between SWCNHs and phytic acid was also confirmed by the analysis of the char residues and gas-phase products. These unique characteristics make the aerogel a promising multifunctional candidate for applications in aviation, aerospace, and other fields.