(1) Background: Photon-counting detector (PCD) CT offers a wide variety of kernels and sharpness levels for image reconstruction. The aim of this retrospective study was to determine optimal settings for coronary CT angiography (CCTA). (2) Methods: Thirty patients (eight female, mean age 63 ± 13 years) underwent PCD-CCTA in a high-pitch mode. Images were reconstructed using three different kernels and four sharpness levels (Br36/40/44/48, Bv36/40/44/48, and Qr36/40/44/48). To analyze objective image quality, the attenuation, image noise, contrast-to-noise ratio (CNR), and vessel sharpness were quantified in proximal and distal coronaries. For subjective image quality, two blinded readers assessed image noise, visually sharp reproduction of coronaries, and the overall image quality using a five-point Likert scale. (3) Results: Attenuation, image noise, CNR, and vessel sharpness significantly differed across kernels (allp< 0.001), with the Br-kernel reaching the highest attenuation. With increasing kernel sharpness, image noise and vessel sharpness increased, whereas CNR continuously decreased. Reconstruction with Br-kernel generally had the highest CNR (Br > Bv > Qr), except Bv-kernel had a superior CNR at sharpness level 40. Bv-kernel had significantly higher vessel sharpness than Br- and Qr-kernel (p< 0.001). Subjective image quality was rated best for kernels Bv40 and Bv36, followed by Br36 and Qr36. (4) Conclusion: Reconstructions with kernel Bv40 are beneficial to achieve optimal image quality in spectral high-pitch CCTA using PCD-CT.