<p>Herein, we reported a Tb-carboxyl-imidazole coordination-crosslinked carboxylated nitrile butadiene rubber (XNBR) elastomer design that exhibits high mechanical robustness, fluorochromism, and white-light emission. Imidazole (Im), a toughening, sensitizing, and self-emissive ligand, highly intensified the fluorescence emission, remarkably toughened the elastomer, and imparted multistimuli responsiveness to the elastomer. The Tb³⁺ ions acted as cross-linking centers and provided high-temperature sensitivity of fluorescence emission (more sensitive than Eu³⁺ ions). The as-prepared XNBR/Tb/Im elastomer, with excellent puncture resistance, exhibited an ultimate extensibility of about 3100% and the highest tensile strength of 22 MPa. Experimental and theoretical investigations have demonstrated that Tb³⁺ ions are more likely to interact with Im ligands with increasing amounts of Im. The number of coordination cross-links with higher cross-linking functionalities showed an increasing trend during stretching. The elastomer exhibited an excitation wavelength and temperature-dependent green emission. By introducing redemissive Eu³⁺ into the elastomer, a white-light-emitting XNBR/Tb/Eu/Im elastomer with chemo-fluorochromism was fabricated. The XNBR/Tb/Eu/Im elastomer exhibited stable white-light emission during both heating and stretching. Changing the temperature only resulted in a variation in the intensity of the white light. We demonstrated the potential applications of these elastomers in patterning and information anticounterfeiting/encryption. This coordination crosslinked tough elastomer with fluorochromism and white-light emission paves a new way to fabricate soft devices and sensors, where optical information displays and optical signal responses are required.</p>