Magnetic Resonance Imaging is perhaps the most important and prominent technique in diagnostic clinical medicine and biomedical research. Its success and development as an imaging technique has been aided by the characteristics of contrast agents that enhance signal intensities and improve specificity. Gadolinium(iii) remains the dominant starting material for contrast agent design but other lanthanide ions (and other oxidation states i.e. +2) are also being increasingly investigated as alternatives to gadolinium(III) within laboratory conditions. This critical review provides a concise summary of the MRI-active gadolinium(III) complexes to date--their pros and cons, an outline of contrast agents based on other lanthanide ions (e.g. europium, dysprosium), and directs the reader to newer, more speculative areas of lanthanide-containing contrast agent design.