The first lanthanide dinitrogen photoswitch [(C 5 Me 4 H) 2 (THF)-Lu] 2 (μ−η 2 :η 2 -N 2 ), 1, is reported. 1 is a unique example of controlled isomerization between side-on and end-on coordination modes of [N 2 ] 2− in a bimetallic lutetium dinitrogen complex that results in photochromism. Near-infrared light (NIR) was used to promote this effect, as evidenced by single X-ray diffraction (XRD) connectivity and Raman data, generating the [N 2 ] 2− end-on bound isomer, [(C 5 Me 4 H) 2 (THF)Lu] 2 (μ−η 1 :η 1 -N 2 ), 2. Although different ligands and coordinating solvents were studied to replicate and control the optical properties in 1/2, only the original configuration with C 5 Me 4 H ligands and THF as the coordinating solvent worked. Supported by the first-principles calculations, the electronic structures along with the mechanistic details of the side-on to end-on isomerization were unraveled. Preliminary reactivity studies show that 2 formed with NIR light reacts with anthracene, generating dihydroanthracene and anthracene dimers, indicating new redox reaction pathways.