3D self-folding microarchitectures have been studied enormously since the past decade, because of the potential of utilizing the third dimension to reach a new level of device integration. However, incorporating various functionalities is a great challenge, due to the limited folding force and choice of materials. In particular, self-folding microarchitectures with advanced optical properties have yet to be demonstrated. Here, a unique folding technique is developed, namely vacuum microforming, successfully demonstrating the self-folding of microcubes that can be completed within 30 ms, a few orders of magnitudes faster as compared to various established strategies reported so far. Simultaneously, a metal–insulator–metal (MIM) plasmonic nanostructure is fabricated, invoking strong gap plasmon to obtain a wide and robust angle-independent optical behavior and high environmental sensitivity that is close to the theoretical limit. It is successfully proven that such superb plasmonic properties are well preserved in 3D architectures throughout the folding process. The nanofabrication method together with the self-folding strategy not only provide the fastest folding process so far, compatible for high-volume fabrication, but also create new opportunities in integrating various functionalities, more specifically, optical properties for untethered optical sensing and identification.