Rhynchophylline (Rhy) is a plant-derived indole alkaloid isolated from Uncaria species. Both the plant and the alkaloid possess numerous protective properties such as anti-inflammatory, neuroprotective, anti-hypertensive, anti-rhythmic, and sedative effects. Several studies support the significance of the anti-inflammatory activity of the plant as an underlying mechanism for most of the pharmacological activities of the alkaloid. Rhy is effective in protecting both the central nervous system and cardiovascular system. Cerebro-cardiovascular disease primarily occurs due to changes in lifestyle habits. Many previous studies have highlighted the significance of Rhy in modulating calcium channels and potassium channels, thereby protecting the brain from neurodegenerative diseases and related effects. Rhy also has anticoagulation and anti-platelet aggregation activity. Although Rhy has displayed its role in protecting the cardiovascular system, very little is explored about its intervention in early atherosclerosis. Extensive studies are required to understand the cardioprotective effects of Rhye. This review summarized and discussed the various pharmacological effects of Rhy in neuro- and cardioprotection and in particular the relevance of Rhy in preventing early atherosclerosis using Rhy-loaded nanoparticles.