Molecular magnetorefrigerant materials for low-temperature magnetic refrigeration and single-molecule magnets for high-density information storage and quantum computing have received extensive attention from chemists and magnetic experts. Lanthanide ions with unique magnetic properties have always been considered as ideal candidates for the construction of such materials. This frontier article focuses on GdIII-based molecular magnetorefrigerants and lanthanide-based single-molecule magnets and highlights the most significant advances.