Aerogels are structural materials with ultralow bulk densities (often less than 0.1 g cm -3 ), which stand out as good candidates for a variety of applications. In the present study, natural rubber (NR)/ clay aerogel composites were produced by freeze-drying of the aqueous aerogel precursor suspensions, followed by solution cross-linking of the aerogel samples in benzene using sulfur monochloride (S 2 Cl 2 ) as a cross-linking agent. The influences of cross-linking conditions, i.e., cross-linker concentration and reaction temperature, as well as polymer loading on the aerogel structure and properties were investigated. 1% (v/v) of S 2 Cl 2 and reaction temperature of -18°C were found to be the optimum conditions for producing a strong and tough rubber composite; the 2.5 wt % NR aerogel, for example, after being cross-linked, exhibited a compressive modulus of 1.8 MPa, 26 times higher than that of the neat control. These favorable mechanical properties are attributed to the high local concentration of rubber and S 2 Cl 2 in the freeze-dried structures, giving rise to the high cross-linking efficiency. Increasing the rubber concentration led to a substantial increase in the mechanical strength, in accord with the changes in microstructure and degree of cross-linking. The swelling capacity of the NR aerogels decreased with either increasing the cross-linker concentration or decreasing the weight fraction of rubber. Cross-linking of the rubber aerogels brought about increased thermal stability, consistent with restricted thermal motion of NR chains.