indispensable, which is ubiquitous in photo nics and optoelectronics applications, such as optical interconnect, environmental monitoring, biosensing, medicine, secu rity, astronomical, and allfibertohome applications. [2,3] Unlike electrons, photons interact weakly with each other. [4] Therefore, an optical modulation requires the media tion of a physical system to produce effi cient photon-photon interactions. Dif ferent approaches to optical modulators have been proposed, often based on fast and highly nonlinear media that would enable alloptical switch devices, including 2D layered materials, [5] high nonlinear responses materials with wellengineered structures, [6] and optomechanical and phasechange metamaterials. [7] However, to our best knowledge, there is no any report about utilizing rare earth (RE) ions to realize fastslow optical modulation. [8,9] Theoretically, it is expected to develop a versatile physical strategy to realize fast slow optical modulation of upconversion (UC) fluorescence from RE ions, which can be tailored by simultaneous twowave length excitation. Among various RE ions, [10][11][12] owing to abun dant energy levels of Ho 3+ ions, it is convenient for us to realize fastslow optical modulation of red UC fluorescence from Ho 3+ ions by simultaneous twowavelength excitation at 1.0 and 2.0 µm lasers. What's more, tunable excitation and emission wavelengths are operating at nearinfrared (NIR) window or atThe control of one light field by another, ultimately at manipulating efficiently photon-photon interactions obsoleting traditional electronic interconnection approach, is an attractive area of research in the development of alloptical network information science. Herein, an exquisite physical strategy is introduced to realize fast-slow optical modulation of red upconversion (UC) fluorescence from Ho 3+ :LaF 3 nanocrystals embedded glass ceramics (GCs) tailoring by simultaneous two-wavelength excitation at 980 and 1870 nm laser. An optical modulation of more than 2500% of the red UC fluorescence intensity and a fast response with rise time of 230 µs and decay time of 66 µs as well as a slow response with rise time of 23 ms and decay time of 6.65 ms in the red UC fluorescence signal is shown. The dynamic evolution analysis and theoretical simulations suggest that this fast-slow optical modulation of red UC fluorescence is rooting from the presence of differentiation of the speed of electrons fully populated in the excited-state 5 I 7 regulated by various pumping tactics. The fast-slow optical modulation of red UC fluorescence from Ho 3+ -doped GCs, manipulating through two-wavelength excitation at 980 and 1870 nm laser, may find novel application in future all-optical fiber data processing in various optoelectronic fields.