Contrast-enhanced magnetic resonance imaging (MRI) is an indispensable tool for diagnostic medicine. However, safety concerns related to gadolinium in commercial MRI contrast agents have emerged in recent years. For patients suffering from severe renal impairment, there is an important unmet medical need to perform contrast-enhanced MRI without gadolinium. There are also concerns over the long-term effects of retained gadolinium within the general patient population. Demand for gadolinium-free MRI contrast agents is driving a new wave of inorganic chemistry innovation as researchers explore paramagnetic transition-metal complexes as potential alternatives. Furthermore, advances in personalized care making use of molecular-level information have motivated inorganic chemists to develop MRI contrast agents that can detect pathologic changes at the molecular level. Recent studies have highlighted how reaction-based modulation of transition-metal paramagnetism offers a highly effective mechanism to achieve MRI contrast enhancement that is specific to biochemical processes. This Viewpoint highlights how recent advances in transition-metal chemistry are leading the way for a new generation of MRI contrast agents.