The combined α-, γ-, and x-ray emitter 213 Bi (half-life, 46 min) is promising for radionuclide therapy. SPECT imaging of 213 Bi is challenging, because most emitted photons have a much higher energy (440 keV) than common in SPECT. We assessed 213 Bi imaging capabilities of the Versatile Emission Computed Tomograph (VECTor) dedicated to (simultaneous) preclinical imaging of both SPECT and PET isotopes over a wide photon energy range of 25-600 keV. Methods: VECTor was equipped with a dedicated clustered pinhole collimator. Both the 79 keV x-rays and the 440 keV γ-rays emitted by 213 Bi could be imaged. Phantom experiments were performed to determine the maximum resolution, contrast-to-noise ratio, and activity recovery coefficient for different energy window settings. Additionally, imaging of [ 213 Bi-DOTA,Tyr 3 ]octreotate and 213 Bi-diethylene triamine pentaacetic acid (DTPA) in mouse models was performed. Results: Using 440 keV γ-rays instead of 79 keV x-rays in image reconstruction strongly improved the resolution (0.75 mm) and contrast-to-noise characteristics. Results obtained with a single 440 keV energy window setting were close to those with a combined 79 keV/440 keV window. We found a reliable activity recovery coefficient down to 0.240 MBq/mL with 30-min imaging time. In a tumor-bearing mouse injected with 3 MBq of [ 213 Bi-DOTA,Tyr 3 ]octreotate, tumor uptake could be visualized with a 1-h postmortem scan. Imaging a nontumor mouse at 5-min frames after injection of 7.4 MBq of 213 Bi-DTPA showed renal uptake and urinary clearance, visualizing the renal excretion pathway from cortex to ureter. Quantification of the uptake data allowed kinetic modeling and estimation of the absorbed dose to the kidneys. Conclusion: It is feasible to image 213 Bi down to a 0.75-mm resolution using a SPECT system equipped with a dedicated collimator. Newoppor tunities for high linear energy transfer radionuclide therapy with the a-particle emitters 225 Ac and 213 Bi are increasingly being investigated (1-3). The research for peptide receptor radionuclide therapy with a-particles is mostly focused on labeling peptides with 213 Bi. Not only is the short half-life of 46 min for 213 Bi in good accordance with the rapid targeting to receptor-positive tumors and the rapid clearance of peptides, it also raises less concern for detrimental effects because of the absence of nonspecific uptake by daughters detached from its peptide or linker due to a-decay recoil (4). 213 Bi offers the best imaging opportunities through its 440 keV g-ray and is therefore important for biodistribution and dosimetry studies (5). All other g-rays and x-rays emitted by 213 Bi and its daughters are too low either in abundance or in energy to be suitable for imaging, possibly with the exception of the x-rays from 213 Bi at 77 and 79 keV if appropriate correction methods for down-scatter of the 440 keV g-rays are applied (Supplemental Table 1; supplemental materials are available at http://jnm.snmjournals.org (6)). Patient imaging of the uptake patte...