This work intends to present a novel numerical approach for studying the vibration behaviours of variable angle tow (VAT) composite structures in their quasi-static nonlinear equilibrium states. This methodology is able to predict the buckling load, to investigate the natural frequencies variation for progressively higher loads, and to provide a means for verifying experimental Vibration Correlation Technique results. The use of VAT composites, in which the fibre orientations are allowed to vary along with a curvilinear pattern within each lamina, dramatically increases the design space and provides a significant improvement in buckling performance and benefits in the postbuckling regime. This study has been performed using an innovative methodology based on the well-established Carrera Unified Formulation able to describe several kinematic models for two-dimensional structures. In detail, layerwise theories are employed to characterize the complex phenomena that may appear in VAT composite structures. All Green-Lagrange strain components are employed because far nonlinear regimes are investigated. Furthermore, the geometrical nonlinear equations are written in a total Lagrangian framework and solved with an opportune Newton–Raphson method along with a path-following approach based on the arc-length constraint. Different VAT composite structures have been analyzed to validate the proposed approach and provide some benchmark solutions. The computed equilibrium paths are compared with results obtained using the commercial code ABAQUS. The results document the good accuracy and reliability of the presented methodology and show this numerical tool’s potentialities.