A wide number of organic and inor ganic materials presents cation exchange properties, such as proteins and poly saccharides, phenolic, acrylic and poly styrene divinyl resins, zeolites, and layered metal oxides. [5,6] Layered titanates are titanium oxide based compounds, with a unique struc ture composed of a 2D host with a guest cation. They have been largely investi gated because of their exchange capacity for application in adsorption of heavy metal ions from water, generation of proton exchange membrane fuel cells or for the synthesis of complex metal oxide structures. [2,[7][8][9] In particular, titanate nanosheets (TNSs) are 2D crystals with a layered nanostructure of [Ti n O 2n+1 ] 2− composition and very small dimension (oneunitcell thickness and 2-6 nm in length). They present good cation exchange properties at the nanoscale because of their high surfacetovolume ratio, the high concentration of hydroxylic groups, and the interlayer distance adaptability. [10][11][12] These nanoparticles have been investigated for the fabrica tion of thin films for optoelectronic applications [13,14] and in combination with a polymeric matrix for the generation of proton exchange membranes. [15] TNSs were combined with silk fibroin (SF) for the fabrication of nanocomposite thin films and membranes with tunable optical properties and processability at the micro and nanoscale range. [16,17] Silk fibroin showed to be an excellent material for the development of biocom patible optical devices and sensors, thanks to its exceptional mechanical and optical properties, associated with biocompat ibility and biodegradability. Many studies have been made on the development of optical and photonic applications based on silk, as microlenses, waveguides, diffraction grating, and inverse opals. [18][19][20][21][22] Recently, researchers have used proteins in combination with 2D nanomaterials (e.g., graphene, dielectric nanosheets, and MXenes) for the generation of nanostructures composites with engineered properties. [23][24][25] These hybrids materials combine the advantages of the biopolymeric matrix, such as biocompatibility and mechanical robustness, with the unique electronic and optical properties of the 2D fillers. In addition, proteins can provide a precise control on the assembly of the material, thanks to the physical and chemical interac tions established with the 2D material. For example, molecular A simple and efficient method is developed to introduce plasmonic and luminescence functionalities in titanate nanosheets (TNSs)-silk nano composites by direct cation-exchange process. First, the cation exchange properties such as exchange kinetic and capacity are studied to verify the behavior of the material and determine the best condition of exchange. In particular, the effect of the valence on the kinetic is investigated through elemental analysis, focusing on three target cations (Ag + , Cu 2+ , and Eu 3+ ) in water. It is demonstrated that the cation exchange capability of the composite is strictly dependent of the amount ...