A novel thermometer, qualified with miniaturization, real-time monitoring, non-invasion, remote-control, and high spatio-temporal resolution, is urgently required for temperaturedetecting of sub-micrometric objects and in specific harsh conditions. Herein, we report an adaptable dual-mode optical thermometry platform LiTaO3:Ti4+, Eu3+@PDMS. A proof-of-concept implementation based on fluorescence thermometer (FT) demonstrates outstanding temperature sensing performance with excellent reversibility. The maximum Sa and Sr are as high as 0.671 and 5.425% K−1, respectively, with minimal temperature resolution of 0.14 K. Whilst, the maximum Sa and Sr based on lifetime thermometer (LT) are determined to be 0.122 and 3.637% K−1, respectively, with superior temperature resolution of 0.027–0.058 K. Finally, flexible phosphor films and 3D micro-rod arrays with handily encrypted information are fabricated for the unclonable multi-modal/multi-dimensional anti-counterfeiting application by exploiting light, temperature and time-domains as the “key” to decrypt the “locked” ciphertext, which indicates the promising prospect in temperature sensing and anti-counterfeiting. This work not only paves a way for developing novel spatial/temporal dual-mode real-time thermometer based on synergetic luminescence of lanthanide (Ln) and transition-metal (TM) ions with high temperature sensitivity and resolution, but also opens a new “window” for extending the thermometer as a flexible device in advanced multi-mode multi-dimensional high-level secure anti-counterfeiting.