The rare-earth metal hydrides with clathrate structures have been highly attractive because of their promising high-[Formula: see text] superconductivity at high pressure. Recently, cerium hydride [Formula: see text] composed of Ce-encapsulated clathrate H cages was synthesized at much lower pressures of 80-100 GPa, compared to other experimentally synthesized rare-earth hydrides such as [Formula: see text] and [Formula: see text]. Based on density-functional theory calculations, we find that the Ce 5p semicore and 4f/5d valence states strongly hybridize with the H 1s state, while a transfer of electrons occurs from Ce to H atoms. Further, we reveal that the delocalized nature of Ce 4f electrons plays an important role in the chemical precompression of clathrate H cages. Our findings not only suggest that the bonding nature between the Ce atoms and H cages is characterized as a mixture of ionic and covalent, but also have important implications for understanding the origin of enhanced chemical precompression that results in the lower pressures required for the synthesis of [Formula: see text].