Over the last decades, interest of researchers in the preparation and study of heterometallic Fe–Ln organometallic compounds has increased due to their intriguing architectures and promising applications as single molecule magnets (SMMs) that exhibit magnetic hysteresis of purely molecular origin. SMMs are fundamentally different from conventional bulk magnets because a collective long-range magnetic ordering of magnetic moments is not necessary. It is expected that SMMs can be employed in the future as the smallest magnetic memory units or in quantum computational devices. This review examines synthetic strategies and magnetic properties of Fe–Ln SMM compounds published till July 2016.