Digital subtraction angiography (DSA) is considered the “gold standard” for the diagnosis of vascular diseases. However, the contrast agents used in DSA are limited to iodine‐based small molecules, which are unsuitable for patients with contraindications. Here, we propose iodine‐free DSA utilizing a bismuth chelate, Bi‐DTPA Dimeglumine, for vascular visualization for the first time. Bi‐DTPA Dimeglumine possesses a simple synthesis process without the need for purification, large‐scale production ability (over 200 g in the lab), superior X‐ray imaging capability, renal clearance capacity, and good biocompatibility. Bi‐DTPA‐enhanced DSA can clearly display the arteries of the rabbit's head and lower limbs, with a minimum vascular resolution of 0.5 mm. The displayed integrity of terminal vessels by Bi‐DTPA‐enhanced DSA is superior to that of iopromide‐enhanced DSA. In a rabbit model of thrombotic disease, Bi‐DTPA Dimeglumine‐enhanced DSA enables the detection of embolism and subsequent reevaluation of vascular conditions after recanalization therapy. Our proposed iodine‐free DSA provides a promising and universal approach for diagnosing vascular diseases.This article is protected by copyright. All rights reserved