Ultrasonic arrays have seen increasing use for the characterisation of composite materials. In this paper, ultrasonic wave propagation in multilayer anisotropic materials has been modelled using plane wave and angular spectrum decomposition techniques. Different matrix techniques, such as the stiffness matrix method and the transfer matrix method, are used to calculate the reflection and transmission coefficients of ultrasonic plane waves in the considered media. Then, an angular decomposition technique is used to derive the bounded beams from finite-width ultrasonic array elements from the plane wave responses calculated earlier. This model is considered to be an analytical exact solution for the problem; hence the diffraction of waves in such composite materials can be calculated for different incident angles for a very wide range of frequencies. This model is validated against experimental measurements using the Full-Matrix Capture (FMC) of array data in both a homogeneous isotropic material, i.e. aluminium, and an inhomogeneous multilayer anisotropic material, i.e. a carbon fibre reinforced composite.