The invention provides methods for delivering a NO molecule or precursor thereof to a vascular compartment of a subject comprising: administering to the subject, a NO particle formulation, via an intravascular, intraperitoneal, or intramuscular administration, in an amount sufficient to induce vascular smooth muscle relaxation thereby delivering the NO molecule or precursor thereof to the vascular compartment of the subject, wherein the NO particle formulation comprises NO attached to a nanoparticle or microparticle.