The effective nonlinear susceptibility X( 3 ) for a composite that consists of a dilute suspension of structured nanoparticles that utilizes the surface mediated plasmon resonance can be enhanced by orders of magnitude compared to the intrinsic X(3) for a film of the same neat material. Here we report calculations for various multilayer spherical nanoparticle models in a host dielectric: i) polymeric core and metallic shell, ii) semiconductor core and metallic shell, iii) metallic core, polymeric shell and metallic second shell, and iv) metallic core, semiconductor shell and metallic second shell. The polymer is polydiacetylene, FDA, the semiconductor is Si, the metal is Ag, and the host is water, a GaAs2 glass or Si. Enhancements as great as 104 can be obtained in both x(3) and the figure of merit with no degradation in the intrinsic speed of the nonlinearity. The choice of geometrical parameters and of component materials permit tailoring of the wavelength dependence and bandwidth characteristics of the nonlinear response. However, fabrication of these structured nanoparticle suspensions remians the key challenge.