Cross-laminated timber (CLT) wall panels are commonly connected to the floor or foundation using metal connections, which play a critical role in determining the seismic performance and energy dissipation of the CLT shear walls. In this study, to comprehend the tension–shear coupling effect of the CLT wall-to-floor angle bracket connections under seismic loads, both monotonic and cyclic shear tests were conducted on the angle brackets that were also simultaneously applied with different levels of prescribed vertical axial tension. The influence of the co-existent axial tension on the horizontal shear performance of the angle brackets was analyzed. Furthermore, a numerical model of the angle brackets was developed and validated with the experimental results, which could predict the tension–shear coupling effect based on the monotonic loading scenario. Based on the numerical model, parametric analysis was conducted, and an analytical tension–shear interaction diagram representing the coupling effect of the angle brackets under seismic loads was established. It is found that with an increase of the axial tension from 0 to 30 kN, the shear resisting capacity of the angle brackets is diminished by 33.29%, and the pinching effect of their hysteretic load–displacement curves is mitigated. When the number of the connection-to-floor screws of the angle brackets was increased from 10 to 14, the shear resisting capacity of the angle brackets can be enhanced by 6.43%, and their shear strength degradation can be relieved by 12.85–56.25%. For the CLT wall-to-floor angle brackets, the analytical interaction diagram can be described using one bilinear function, which consists of the ratio between the shear to the shear resistance and the ratio between the tension to the pull-out resistance.