The invention provides NO-releasing polymers and low molecular weight NO-releasing compounds which may be used to for the treatment of medical conditions associated with NO-deficiency. The NO-releasing polymers or the low molecular weight NO-releasing compounds may also be incorporated into medical devices. The invention further provides methods of controlled release of NO for the treatment of diseases and disorders associated with NO-deficiency, wherein the treatment includes systemic or local administration of the NO-releasing polymers or the low molecular weight NO-releasing compounds.