Constrained layer damping (CLD) structures, which are one of the composite structures with a softer viscoelastic material (VEM) layer sandwiched between a elastic base layer and a relatively stiffer constraining layer, are widely used in engineering applications for reducing vibration and noise radiation. To accurately predict and effectively control vibration and properly and quickly determine the design parameters, optimal designs for the CLD structures are necessary. The optimal designs depend on thoroughly understanding the damping characteristics of the CLD structures. In addition, for some cases, CLD structures with multi-constrained VEM layers are needed to suppress vibration more effectively. In this paper, an effective modeling method to accurately describe the damping properties and a quick optimization design method using COMSOL were proposed for CLD structures with multilayers in detail. The effects of nondimensional thickness ratios of the VEM and constraining layer to the base layer on the damping properties of CLD structures were analyzed. For CLD structures with different configurations, different constraints were selected to obtain the maximized damping in the optimization design. The conclusions from this research provide an insight into the effects of thicknesses of VEM and constraining layers on the damping properties of CLD structures regardless of its size. The modeling and optimal methods using COMSOL in this paper are not limited to CLD structures and can be used by other structures also.