Reduction of radar cross section (RCS) for targets can be achieved by different approaches and coating absorbing materials at the surfaces of targets is one of widely used methods because of its flexibility and good effect. In the work, we put forward a novel method of reducing the RCS based on the design of multilayer composite absorbing materials. The transmission line theory and particle swarm optimization (PSO) are used to guide the design and analysis, and two kinds of designs, i.e., Type IV and Type VII, are selected finally. Simulation experiments show that the designs are insensitive to the incident angles and polarizations of incident EM wave, which is required for being coated at the surfaces of real objects. Also, the designed absorbing materials are very thin and have an ultra-wide frequency band. The bandwidth of Type-IV design can reach 14.6314.63 GHz, ranging from 3.373.37 to 18.018.0 GHz, while Type-VII design can cover the frequency range from 2.02.0 to 18.018.0 GHz, which represents the major part of radar’s frequency range. The designed absorbing materials are coated at the surface of a perfectly-electric-conducting (PEC) cylinder to validate the effectiveness of the materials, and good results have been obtained.