Angiogenesis and inflammation are clearly interconnected and interdependent processes that are dysregulated in a series of systemic and brain pathologies. Herein, key aspects regarding endothelial cell function and tissue remodelling that are particularly affected or aggravated by inflammation are presented. Most importantly, the cellular and molecular mechanisms involved in the vascular regulation of the inflammatory processes occurring in several brain disorders and how they impact on disease/injury progression are detailed, highlighting potential targets for therapy. Finally, nanomedicine-based approaches designed to overcome limitations pertaining to low systemic bioavailability, light, pH and temperature sensitivity and/or rapid degradation of these targets, and to optimize their mode of action are discussed. Ultimately, we expect this review to provide new insight and to suggest novel approaches for the treatment of blood–brain barrier dysfunction per se or as a means to treat the injured or diseased central nervous system.