The theological properties and mechanical properties of percolated cyanate ester monomer/layered silicate mixtures are reported. A number of different cation exchanged montmorillonites were examined in an effort to achieve maximal montmorillonite delamination. The dispersion throughout the cyanate ester of a montmorillonite with phenylated ammonium cations (2MBHT MMT) results in the formation of a percolated network. The rheology of this percolated network undergoes a viscous liquid to elastic solid transition at 4 wt% montmorillonite. The percolation of the montmorillonite in the cyanate ester results in a significant improvement in crack resistance (80%) without a sacrifice of flexural strength. (c) 2005 Elsevier Ltd. All rights reserved.