Myocardial perfusion scintigraphy was performed with both 201Tl and a new six coordinate monocationic isonitrile complex of 99mTc, [99mTc]2-methoxyisobutylisonitrile (MIBI), on 11 infants who had undergone the arterial switch procedure for transposition of the great arteries. Unlike 201Tl which can show rapid and variable rates of washout from myocardium, 73% of the initial first-pass activity of the isonitrile complex in the myocardium remains 1 hr after intravenous administration. The images obtained with [99mTc]MIBI required a shorter recording time, entailed less radiation exposure to the patient, and were qualitatively at least as good as those obtained with 201Tl. No infant had perfusion abnormalities. The potential applications of the isonitrile complexes for myocardial perfusion scintigraphy in children are discussed.