The preparation and modification of crystal structures in cryogenic environments with conventional methods is challenging, but it is essential for the development of composite materials, energy savings, and future human space exploration. Plasmon induced hot carriers and local thermal effects help to overcome the challenges of chemical reactions under extreme conditions, for which molecular reactions have attracted considerable research attention. In this work, the plasmon thermal effect enables fast and efficient nanocrystal transformation in cryogenic environments, which was previously unattainable with conventional heating methods. The transformation of NaYF4 nanocrystals on gold nanoparticle island films can be achieved even in a low temperature environment of 11 K. Compared with the structure with gold nanoparticles adhered to NaYF4 nanocrystals directly, the structure of gold nanoparticle island films with an Al2O3 layer offered better heat trapping properties, which allows the complete transformation to take place of NaYF4 nanocrystals into Y2O3 nanocrystals in low temperature environments. This work explores the potential of applying the photothermal effect of a plasmon to induce rapid transformation of nanocrystals in extreme environments and provides insight into the process of crystal transformation and growth.