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The correct choice for a vasodilator primarily used to dilate coronary arteries and treat angina is nitroglycerin. Nitroglycerin works by relaxing smooth muscle in blood vessels, leading to dilation, particularly in the coronary arteries. This dilation increases blood flow to the heart muscle, thus relieving the ischemia that can cause angina.

Diltiazem, on the other hand, is a calcium channel blocker that does have some effects on coronary artery dilation and can help with angina by decreasing heart rate and myocardial contractility. However, its primary mechanism does not specifically focus on dilating coronary arteries as the main treatment for angina.

Captopril is an ACE inhibitor, primarily used for heart failure and hypertension, and does not specifically target coronary artery dilation.

Sodium nitroprusside is a potent vasodilator used primarily in acute settings to rapidly lower blood pressure and is not typically used for the treatment of angina in a chronic setting.

Thus, while diltiazem has a role in angina management, nitroglycerin is specifically recognized for its effectiveness in dilating coronary arteries to treat angina symptoms.