90Y bremsstrahlung Single-Photon Emission Tomography (SPECT) imaging is employed to check the possibility of extrahepatic uptake and the quantification of delivered dose in Transarterial Radioembolization (TARE). 90Y bremsstrahlung SPECT imaging is challenging due to the nature of bremsstrahlung photons. We reported a Monte Carlo study using the resin microspheres loaded with 90Y and Nanoparticles (NPs) in the TARE. By injection of Bismuth (Bi) and Europium (Eu) NPs into the resin microspheres, the sensitivity and the contrast to noise ratio increased for the bremsstrahlung planar images. The highest signal to background ratio was observed in the characteristic X-ray planar images taken with the energy window at the Kα1 ± 10 keV when Eu NPs were incorporated into the microsphere. The dose enhancement ratio decreased dramatically at NP concentrations >2.4 M. Incorporating NPs into the resin microspheres improves the quality of post-treatment images and establishes a standardized imaging protocol for post-treatment imaging by characteristic X-rays.