Optimized lightweight, compact and high temperature sustaining shielding materials for neutron and gamma radiation were developed by genetic algorithms (GA) combined with the Monte Carlo N-Particle (MCNP) code. A series of samples were designed according to the method. Deep penetration tests by the MCNP code were completed. The results show that the designed samples have more advantages related to the radiation shielding effects in comparison with PB202 and KRAFTON-XP3, especially the Cakes with multi-layers structures of the Fe-interlayer-Pb have excellent performance. Taking into account the ratios designed of components among elements in the material, the manufacturing process of polymer with nano-TiO2 was studied experimentally by differential scanning calorimetry (DSC). Several samples have been tested. The attenuation experiments on the samples were carried out using tandem electrostatic accelerator neutron source, spontaneous fission neutron source of 252Cf and gamma-rays source of 60Co. The experimental results verify the correctness of optimal design and craft. The Cakes are quite suitable for applications in the practices of nuclear science and technology.