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Although various fabrication methods for metal–oxide nanostructures have been well developed for enlarged surface area, numerous efforts to further enhance the effective surface area for their chemical sensor applications are still being studied. Herein, a high‐power laser is irradiated on the existing metal–oxide nanostructures to expose the hidden inner surface of the nanostructures for full participation in the surface gas‐sensing reactions, resulting in extraordinary gas‐sensing performance. In addition, noble metal catalyst decoration at both the inner and outer surfaces of the nanostructures records extremely high gas response and selectivity to volatile organic compounds. The numerical simulation and experimental verification of the effects of high‐power laser irradiation for morphological evolution of the metal–oxide nanostructures can provide a new perspective toward the time‐efficient development of nanostructure‐based electronic devices.