Millions of individuals worldwide are affected by the common and deadly condition of hypertension. Despite the availability of several antihypertensive medications, researchers continue to look for new and potent treatments. Because of their eco-friendliness and simplicity of scaling, pyrimidine-based compounds have demonstrated potential antihypertensive efficacy. Recent developments in the green synthesis of pyrimidine compounds and their antihypertensive efficacy are highlighted in this review. The pharmaceutical business and the environment may be significantly impacted by the adoption of sustainable and green chemical methodologies in the synthesis of innovative antihypertensive drugs.