摘要：The realization of tunable nonlinear optical(NLO)responses in a single nano-/micro-structure is extremely ***,in lack of effective ways to integrate multiple performances,it still faces severe limitations during ***,we demonstrate a wavelength-dependent NLO micro-structure based on host-guest metal-organic framework(MOF)materials through encapsulating linear dye molecules into periodic one-dimensional(1D)*** confinement to non-centrosymmetric polar dye molecules enhances the second-/third-order NLO responses of the hybrid crystals,causing obvious two-photon luminescence(TPL),second harmonic generation(SHG)and third harmonic generation(THG)responses in the as-prepared *** highly ordered structures of MOFs impart spatial regulation on the linear dye molecules to realize orientation alignment,resulting in the polarized anisotropy ***-to-NIR(NIR,near-infrared region)two-photon pumped lasing is realized with the natural whispering gallery mode resonance cavities of MOFs under the excitation of a 1200-nm fs ***,tunable NLO properties such as TPL,SHG and THG are achieved through switching the incident excitation wavelength from 800 to 1500 *** hybrid materials with tunable NLO responses may open a new avenue toward designing multifunctional NLO devices in the future.