The artificially periodic structures with the bandgap (BG) features provide a fantastic way for elastic wave manipulation. However, omnidirectional control of elastic waves at low-frequency remains a challenge, especially in the engineering application, due to the great different material parameters of the structure's components. In this work, we present the design of a three-dimensional syndiotactic metastructure (STM) and isotactic metastructure (ITM) composed of a single material with the same density and stiffness. A low-frequency broad bandgap occurs in the global band structure of STM. Meanwhile, it also retains the same high-frequency ultra-wide BG as that of ITM. The formation of the low-frequency BG of STM is attributed to the simultaneous activation of rotation and translation modes. The static deformation analysis indicates that STM has a unique translational and rotational coupling mechanism. The frequency response results reveal that the coupling mechanism can also enhance the attenuation of high-frequency BG.