photonics and optoelectronics is the lack of materials with broad-band optical response and strong light-matter interaction. Therefore, it is an urgent need and many efforts have been devoted to searching for this kind of novel materials. [2][3][4][5] The broad-band optical response of 2D nanomaterial is related to the unique band structure and electronic properties. [1] Graphene exhibits a wide-spectral photonic response from ultraviolet to the radio-wave regimes owing to its gapless and conical-shape band structure. However, lack of intrinsic bandgap makes graphene-based devices suffer from relatively small on/off ratio, large dark current, and poor photo response. The relative low absorption and high non-saturable loss of graphene in optical response limit its extensive applications. [6][7][8][9] Following graphene, the most studied 2D transition metal dichalcogenides (TMDCs) possess a bandgap ranging from 1.0 to 2.0 eV, indicating their practical optoelectronic applications are not available in midinfrared (MIR) wavelength range. [10,11] After graphene and TMDCs, black phosphorus (BP), the most thermodynamically stable allotrope of phosphorus, has been thoroughly studied as a novel 2D layered material since early 2014. [12] It has triggered significant interests in both scientific research and potential electronic, optoelectronic, and biomedicine applications because of its unique and exotic properties. [13][14][15] Layered BP has a direct bandgap with layer-dependent variation over ≈0.3-2.0 eV, which gives rise to broad-band optical properties from visible to MIR region. The intrinsic layer-dependent direct bandgap gives rise to high on/off ratio and low dark current for electronic devices and makes BP an appropriate 2D material for MIR photonic applications. Moreover, the bandgap of BP can be efficiently tuned by electrical gating, which should pave the way for optoelectronic devices. [16] BP presents puckered structure with in-plane anisotropy, which results in specific dichroic optical properties of light absorption and photoluminescence. [17] However, easy oxidation under ambient environment is the biggest obstacle that significantly impedes its practical applications. [14,[18][19][20][21][22] Therefore, how to improve the long-term stability of BP has become a challenge.Germanium phosphide (GeP), a typical 2D group IV-V semiconductor, has attracted significant attention due to the advantages of higher thermodynamic stability than black phosphorus (BP), widely tunable bandgap, high carrier mobility, and in-plane anisotropy. However, its photonic and optoelectronic properties have not been extensively explored so far. Herein, large size and high-quality GeP single bulk crystal is successfully grown by flux method and stripped into 2D nanosheets with liquid phase exfoliation (LPE) and spin-coating methods. The broad-band photonic and optoelectronic properties of 2D GeP nanosheets are systematically investigated. First principles calculations are performed to verify its widely tunable bandgap from 0.43 eV f...