The mechanical properties of carbon fiber sheet molding compounds (CF-SMCs) are sensitive to the internal geometry of the reinforcing fibers. In this study, novel CF-SMCs with outstanding mechanical performance, namely, chopped carbon fiber tapes reinforced thermoplastics (CTTs), were fabricated using tapes with different thicknesses. The effects of the tape morphology on the tensile properties of the CTTs were evaluated both experimentally and analytically. Two X-ray-aided computed tomography (CT) based methods were adopted to analyze the effects of the tape thickness on the internal geometry of the CTTs. The modified Mori-Tanaka model was used based on the fiber orientation data obtained from the X-ray micro-CT analyses. The results showed that the tensile properties decreased significantly with an increase of the out-of-plane misorientation, which is more intensive for thicker tapes. In addition, the tensile properties showed greater variations as the tape thickness was increased. The two X-ray micro-CT methods were found to be suitable for visualizing and quantitatively analyzing the internal geometries. Correlations were found between the tape thickness and the tensile properties. Finally, the results of the simulations performed using the Mori-Tanaka model and the fiber orientation data were found to be similar to those of the experiments in tensile moduli, but the results for strength deviate from the experiments.