The increased utilization of high power laser sources has rendered great challenges for designing effi cient optical limiting (OL) materials to protect human eyes and various delicate optical devices. An ideal optical limiter should greatly attenuate an intense laser beam while exhibiting high transmittance for low-input optical intensity. [ 1 ] Up to now, numerous organic and inorganic materials have proved to be good candidates for optical limiters with different working mechanisms. Among them, carbon-based materials, such as fullerenes, carbon black, and carbon nanotubes, have exhibited very good OL performance. [2][3][4][5] As a typical representative, graphene, which consists of sp 2 -hybridized carbon atoms with single-atom thickness and 2D structure, has exhibited unique electronic, optical, and mechanical properties. [ 6 ] The interband optical transitions in graphene are independent of frequency over a wide range and depend only on the fi nestructure constant, thus it is naturally promising as a broadband optical limiter. [ 7 ] Another important advantage of graphene-based materials is that they can be easily functionalized with organic molecules and hybridized with inorganic nanomaterials via covalent bonding, to improve their OL performances through the synergistic effect. For example, the enhanced nonlinear optical properties have been reported in porphyrin-functionalized graphene, [ 8 ] organic dye ionic complex, [ 9 ] oligothiophene, [ 10 ] fullerene, [ 11 ] phthalocyanine, [ 12 ] and CdS quantum dots. [ 13 ] We have noticed that all the OL properties of graphenecontaining materials, usually dispersed in liquid media, have been studied only under nanosecond excitation conditions and the working wavelengths of the lasers used are mainly 532 or 1064 nm. [7][8][9][10][11][12][13] However, the studies on the OL properties of graphene-containing materials in femtosecond region and other wavelengths are still absent. To a large extent, it may be due to the saturable absorption behavior of graphene under the excitation of femtosecond laser with low frequency. [ 14 , 15 ] Though most of the materials reported have shown good OL behavior in the nanosecond region due to the dominance of nonlinear scattering (NLS), they suffer from the dramatic decrease of OL performance due to the strongly suppressed NLS effect when fabricated into solid fi lms or excited with femtosecond pulse, which remains a serious obstacle for real applications. Therefore, design and synthesis of novel graphene-based OL materials that can work in the femtosecond pulse domain and other wavelengths region still represents a signifi cant challenge.Due to the long lifetime (in the order of milliseconds) of their real metastable states, upconversion process of lanthanide (Er 3 + , Yb 3 + , and Tm 3 + ) ions doped in the lattice of NaYF 4 nanocrystals after near infra-red (NIR) laser excitation, can be nearly 10 5 times more effi cient than the typical twophoton absorption process observed in organic molecules. [ 16 ] Therefore, it is highly...