Metal-organic frameworks (MOFs) are a fascinating class of structured materials with diverse functionality originating from their distinctive physicochemical properties. This review focuses on the specific chemical design of geometrically frustrated MOFs along with the origin of the intriguing magnetic properties. We have discussed the arrangement of spin centres (metal and ligand) which are responsible for the unusual magnetic phenomena in MOFs. Both two-dimensional (2D) and three-dimensional (3D) MOFs with frustrated magnetism, their synthetic routes, and evaluation of magnetic properties are highlighted. Such spin-frustrated MOFs may find applications in the field of memory devices, transistors, sensors, and the development of unconventional superconductors.