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 (S2Cl2) 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 S2Cl2 and reaction temperature of 18 degrees 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 S2Cl2 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.