The mechanical behaviour of unbonded post-tensioned (UPT) shear walls of high-strength CAlcium SIlicate ELement masonry with Thin-Layer Mortar (CASIEL-TLM masonry) was investigated experimentally and numerically. Eight walls were tested with the following key variables: unit type, prestress level and cross-sectional shape (rectangular or T-shaped with interlocking of web and flange). An extensive measurement scheme was adopted that allowed derivation of average curvatures and strains in the bottom region of the wall in addition to wall displacements. Since UPT masonry is characterised by the absence of local compatibility between masonry and the UPT tendons, a numerical model for quasi-static, monotonic push-over analysis was developed that provides an iterative solution for the global interaction between masonry and UPT tendons. A common masonry stress–strain diagram was adopted in the numerical model. A peculiarity of CASIEL-TLM masonry is the kicker course, which reduces the stiffness of the bottom region of the shear wall. This layer was modelled with no-tension, linear-elastic behaviour and a reduced stiffness. Nevertheless, the model underestimates the experimental deformations of the rectangular shear walls, while the strength is in reasonable agreement. The walls with T-shaped crosssection failed prematurely by shear of the web-flange interface, resulting in diagonal splitting cracks in the interlocking units. This paper deals with the experimental results of UPT CASIEL-TLM masonry shear walls with rectangular and T-shaped cross-section and with the numerical modelling of the overturning behaviour of UPT shear walls with rectangular cross-section.