Background Photon-counting CT (PCCT) represents a recent advancement in CT, offering improved spatial resolution and spectral separability. By using multiple adjustable energy bins, PCCT enables K-edge imaging, allowing mixed contrast agent distinction. Deep-silicon is a new type of photon-counting detector with different characteristics compared with cadmium photon-counting detectors. Purpose To evaluate the performance of a prototype deep-Si PCCT scanner and compare it with that of a state-of-the-art dual-energy energy-integrating detector (EID) scanner in imaging coronary artery plaques enhanced with iodine and K-edge contrast agents. Materials and Methods A series of 10 three-dimensional-printed inserts (diameter, 3.5 mm) was prepared, and materials mimicking soft and calcified plaques were added to simulate stenosed coronary arteries. Inserts filled with an iodine- or gadolinium-based contrast agent (GBCA) were scanned. Virtual monoenergetic images (VMIs) and iodine maps were generated using two- and eight-energy bin data from EID CT and PCCT, respectively. Gadolinium maps were calculated for PCCT. The CT numbers of VMIs and iodine maps were compared. Spatial resolution and blooming artifacts were compared on the 70-keV VMIs in plaque-free and calcified coronary arteries. Results No evidence of a significant difference in the CT number of 70-keV images was found except in inserts containing GBCAs. In the absence of a GBCA, excellent (r > 0.99) agreement for iodine was found. PCCT could quantify the GBCA within 0.2 mg Gd/mL ± 0.8 accuracy of the ground truth, whereas EID CT failed to detect the GBCA. Lumen measurements were more accurate for PCCT than for EID CT, with mean errors of 167 versus 442 µm (P < .001) compared with the 3.5-mm ground truth. Conclusion Deep-Si PCCT demonstrated good accuracy in iodine quantification and could accurately decompose mixtures of two contrast agents. Its improved spatial resolution resulted in sharper images with blooming artifacts reduced by 50% compared with a state-of-the-art dual-energy EID CT scanner. © RSNA, 2024.