Image-based computational tools could enable physicians to personalize and optimize intra-arterial drug delivery and predict outcomes before administering treatments. Tailoring the drug delivery process to the specific attributes of each individual can significantly improve the overall efficacy and safety of the treatment. This chapter describes a patient-specific computational model developed to support the design of intra-arterial nanoparticulate drug delivery systems and advance our understanding of the complex interface between the physicochemical properties of the drugs delivered and the local physiological factors at play. Results of our in silico analysis show that the patient’s vascular architecture, local hemodynamics, and disease state, along with drug design parameters, including particle size and surface characteristics, influence the vascular deposition pattern of nanomedicine.