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Abstract Increasing interests in stretchable electronic devices have resulted in vigorous research activities, most of which are focused on structural configurations. Diverse structural configurations are available for stretchability, including stiff-island, serpentine, and buckled structures. With easily deformable shapes and simple fabrication processes, buckled structures have the potential to realize stretchability. However, conventional buckled structures exhibit stretchability only in a single-axis direction. In the present study, a new type of cross-buckled structure, which can overcome the limitations of conventional buckled structures is developed. The stretchable thin film solar cells with the cross-buckled structure showed stable mechanical and electrical characteristics under both stretching and compressing conditions. The cross-buckled structure for stretchable electronic devices is expected to broaden the fields of wearable electronics, stretchable displays, and biocompatible applications.