An effective method to design structural Left-handed material(LHM) was proposed. A commercial finite element software HFSS and S-parameter retrieval method were used to determine the effective constitutive parameters of the metamaterials, and topology optimization technique was introduced to design the microstructure configurations of the materials with desired electromagnetic characteristics. The material considered was a periodic array of dielectric substrates attached with metal film pieces. By controlling the arrangements of the metal film pieces in the design domain, the potential microstructure with desired electromagnetic characteristics can be obtained finally. Two different LHMs were obtained with maximum bandwidth of negative refraction, and the experimental results show that negative refractive indices appear while the metamaterials have simultaneously negative permittivity and negative permeability. Topology optimization technique is found to be an effective tool for configuration design of LHMs. An effective method to design structural Left-handed material (LHM) was proposed. A commercial finite element software HFSS and S-parameter retrieval method were used to determine the effective constitutive parameters of the metamaterials, and topology optimization technique was introduced to design the microstructure configurations of the materials with desired electromagnetic characteristics. The material considered a a periodic array of dielectric substrates attached with metal film pieces. By controlling the arrangements of the metal film pieces in the design of the film The two different LHMs were obtained with maximum bandwidth of negative refraction, and the experimental results show that negative refractive indices appear while the metamaterials have simultaneously negative permittivity and negative permeability. Topology optimization technique is found to be an effective tool for config uration design of LHMs.