Background: The technological developments for nanocellulose production from cheaper plant materials compared to wood, in particular, agricultural waste is an urgent task of nanobiophysics. The discovery of possibility of expanding the functional characteristics of materials in compositions with modified cellulose particles essentially stimulated the interest of researchers in cellulose composites. Surface modification of cellulose particles by functional materials, such as dyes, metal oxides, silicon, allows applying composites with modified cellulose in various areas of modern industry. A significant improvement in the operational performances of functionalized cellulose particles can be achieved by using them as filler in polymers. Epoxy resin compositions with modified and unmodified cellulose particles, studied in present work, are an example of hybrid biosystem. The interfacial interaction of filler particles with the epoxy matrix, their concentration and dispersion can change the physical and chemical properties of the biopolymer and the functional parameters of biocomposites. Studying the influence of external fields on the physical and chemical properties of epoxy resin-based biosystems and their influence on operational parameters seems to be an urgent problem of advanced and sustained materials science. Objectives: The purpose of this work was to develop an effective nanocellulose synthesis from plant materials and surface functionalization of micro- and nanocellulose particles with clathrochelate iron (ΙΙ) dye as well obtaining biocompositions of epoxy resin with functionalized and non-functionalized micro- and nanocellulose, and to explore of the morphology, chemical resistance, mechanical and thermal properties of epoxy composites with cellulose micro and nanoparticles. Materials and methods: The studying objects were the composites of epoxy resin Eposir-7120 with a polyethylene polyamine “PEPA” hardener in a ratio of 6.2:1 and 10% cellulose micro and nanoparticles. The microcellulose obtained from wood has been a commercial product. Nanocellulose has been synthesized from organosolv cellulose obtained from Miscanthus x giganteus stalks. Surface modification of micro- and nanocellulose was performed using the clathrochelate iron (ΙΙ) dye. The specific surface area of cellulose particles was determined using low-temperature nitrogen adsorption-desorption according to the Brunauer-Emmett-Teller method. Mechanical parameters were determined using universal Shopper and UMM-10 machines. Thermal analysis was performed using Q1500 analyzer. Swelling was determined by the gravimetric method. Results: Elastic modulus E, compressive strength σ and thermogravimetric parameters were determined. It was shown that in composites with micro and nanocellulose the E rises in 7.0–12.2% while the σ increases in 9.1% for composites with cellulose micro particles. The loading resin with nanocellulose and modified cellulose microparticles no affects the σ value of composites. The thermal stability of epoxy polymer (310°C) reduces after loading with micro and nanocellulose to 290 and 300°C, respectively. Chemical resistance of composites with both celluloses to 20% nitric acid reduces. In neutral medium swelling characterizes by rapid sorption to saturation of 15–20% acetone in 36 hours. Conclusions: Thus, the synthesis method of nanocellulose from plant materials and functionalization of its surface with clathrochelate iron (ΙΙ) were developed. Light response of dye was detected in visible spectral range. Epoxy resin composites with 10% micro and nanocellulose were obtained. The filling effect with micro- and nanocellulose at elastic modulus, compressive strength, and thermal stability of epoxycomposites was studied. The swelling processes run similarly in composites with cellulose micro and nanoparticles.