Molecular imaging refers to the non-invasive visualisation of biological processes at the molecular and cellular levels within a living organism, and offers a wide range of potential benefits to both clinical medicine and research into novel therapeutic agents. Inflammation plays an important role in a wide variety of pathological processes and imaging the molecular and cellular machinery that underlies chronic inflammation is attractive and feasible. In this review, we present an overview of molecular imaging of inflammation. We start by characterising molecular and cellular events in early inflammation, identifying current and potential future imaging targets. We focus on the imaging of endothelial cells, which mediate the important first steps in inflammation in any tissue, are readily accessible to imaging probes and which present an approach that can be applied across multiple modalities. We then review the generic requirements for imaging contrast agents and focus on the important considerations in respect of ligands, ligand-target interactions and contrast vehicles. We aim to provide an integrated view of current progress with a focus on promising recent developments in experimental and translational molecular imaging.