A composite material that leads to self organization of mesogen-coated gold nanospheres is synthesized and shows enhanced anisotropic optical properties due to synergistic effects of the mesogens intrinsic birefringence and its ability to drive the self-assembly process into highly anisotropic architectures with densely packed nanospheres. Such nanoengineered matter sustains a response beyond that achievable by its individual constituents, i.e., a metamaterial.