Radiation causes damage to the human body, the environment, and electronic equipment. Shielding against neutron and gamma rays is particularly difficult because of their strong ability to penetrate materials. Conventional gamma ray shields are typically made of materials containing Pb. However, they pose problems in that Pb is a heavy metal, and human poisoning and/or pollution can result from the manufacturing, use, and disposal of these materials. In addition, neutron rays are shielded by materials rich in H2 or concrete. In the case of the latter, the manufacturing cost is high. Thus, it is necessary to develop a new multilayer structure that can shield against both neutron and gamma rays. We set up a simulation model of a multilayered structure consisting of metal hydrides and heavy metals, and then evaluated the simulations using Monte Carlo N-Particle Transport Code. Monte Carlo simulation is an accurate method for simulating the interaction between radiation and materials, and can be applied to the transport of radiation particles to predict values such as flux, energy spectrum, and energy deposition. The results of the study indicated the multilayer structure of ZrH2, U, and W could shield both neutron and gamma rays, thus showing potential as a new shielding material to replace Pb and concrete.