The evaluation of radiation absorbed doses in tumorous and healthy tissues is of increasing interest for 90 Y microsphere radioembolization of liver malignancies. The objectives of this work were to introduce and validate a new reconstruction method for quantitative 90 Y bremsstrahlung SPECT to improve posttreatment dosimetry. Methods: A fast Monte Carlo simulator was adapted for 90 Y and incorporated into a statistical reconstruction algorithm (SPECT-MC). Photon scatter and attenuation for all photons sampled from the full 90 Y energy spectrum were modeled during reconstruction by Monte Carlo simulations. The energy-and distance-dependent collimator-detector response was modeled with precalculated convolution kernels. The National Electrical Manufacturers Association 2007/International Electrotechnical Commission 2008 image quality phantom was used to quantitatively evaluate the performance of SPECT-MC in comparison with those of state-of-the-art clinical SPECT reconstruction and PET. The liver radiation absorbed doses estimated by SPECT, PET, and SPECT-MC were evaluated in 5 patients consecutively treated with radioembolization. Results: In comparison with state-of-the-art clinical 90 Y SPECT reconstruction, SPECT-MC substantially improved image contrast (e.g., from 25% to 88% for the 37-mm sphere) and decreased the mean residual count error in the lung insert (from 73% to 15%) at the cost of higher image noise. Image noise and the mean count error were lower for SPECT-MC than for PET. Image contrast was higher in the larger spheres (diameter of $28 mm) but lower in the smaller spheres (#22 mm) for SPECT-MC than for PET. In the clinical study, mean absorbed dose estimates in liver regions with high absorbed doses were consistently higher for SPECT-MC than for SPECT (P 5 0.0625) and consistently higher for SPECT-MC than for PET (P 5 0.0625). Assessment of the 90 Y microsphere distribution can be performed by imaging bremsstrahlung photons with a SPECT camera or by imaging annihilation photons with a PET camera. Posttreatment dosimetry with 90 Y PET has advantages over SPECT, mainly because of higher resolution and image contrast (6,7). However, the low positron branch (32 · 10 26 ) in 90 Y decay requires a stateof-the-art lutetium-(yttrium)-orthosilicate time-of-flight PET/CT scanner to obtain images with sufficiently high quantitative accuracy for dosimetry purposes (8,9). Posttreatment imaging with a standard SPECT/CT system may be a more widely available and cost-effective option for most centers, but the image quality (IQ) of state-of-the-art clinical 90 Y bremsstrahlung SPECT is still limited (7). The wide range (0-2.3 MeV) and continuous nature of the 90 Y bremsstrahlung photon spectrum prohibit the use of simple energy window-based scatter rejection and correction techniques, hinder attenuation correction based on single-photon energy, and require compensation for collimator-and detector-related imagedegrading effects, such as collimator scatter, lead x-rays, septal penetration, camera (back)scatter, an...