Nondestructive methods, to calculate the buckling load of imperfection sensitive thin-walled structures, such as large-scale aerospace structures, are one of the most important techniques for the evaluation of new structures and validation of numerical models. The vibration correlation technique (VCT) allows determining the buckling load for several types of structures without reaching the instability point, but this technique is still under development for thin-walled plates and shells. This paper presents and discusses an experimental verification of a novel approach using vibration correlation technique for the prediction of realistic buckling loads of unstiffened cylindrical shells loaded under axial compression. Four different test structures were manufactured and loaded up to buckling: two composite laminated cylindrical shells and two stainless steel cylinders. In order to characterize a relationship with the applied load, the first natural frequency of vibration and mode shape is measured during testing using a 3D laser scanner. The proposed vibration correlation technique allows one to predict the experimental buckling load with a very good approximation without actually reaching the instability point. Additional experimental tests and numerical models are currently under development to further validate the proposed approach for composite and metallic conical structures.