Helium-3 (3He) is a noble gas that has critical applications in scientific researches and promising application potential as clean fusion energy. It is thought that the lunar regolith contains large amounts of helium. But it is challenging to extract because most helium atoms are reserved in defects of crystals or as solid solutions. Here, we find large amounts of helium bubbles in the glassy surface layer of ilmenite particles that were brought back by Chang’E-5 mission. The special disorder atomic packing structure of glasses should be the critical factor for capturing the noble helium gas. The reserves in bubbles don’t require heating to high temperatures to extract. Mechanical methods at ambient temperatures can easily break the bubbles. Our results provide insights on the mechanism of helium gathering on the moon and offer guidance on future in situ extraction of helium on the Moon.