Albumin is a macromolecule that remains largely confined to the vascular space after intravenous administration. Human serum albumin was paramagnetically labeled by covalently binding from nine to 18 gadolinium-DTPA (diethylenetriaminepentaacetic acid) chelates per protein molecule. This conjugate was tested in varying doses for in vivo biodistribution and effectiveness in tissue relaxation. After intravenous injection of the agent in rats, T1 relaxation times were significantly reduced in samples of the blood and in lung, heart, spleen, kidney, and brain tissue. These effects persisted at a relatively constant level for the next 30 minutes. In vivo magnetic resonance imaging of the heart and lungs of rats and rabbits confirmed the prolonged contrast-enhancing effect of the labeled albumin. These preliminary studies indicate that paramagnetically labeled macromolecules that distribute in the intravascular space may be effective for MR imaging evaluation of tissue blood volume.