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Fibrillated celluloses have gained significant attention due to their exceptional mechanical properties and eco-friendly characteristics, which make them suitable for various applications. In this study, we designed a precise approach for producing highly fibrillated microcrystalline cellulose (MCC) via ball-milling treatment using four typical silane coupling agents. The empirical data demonstrate that the fibrillization of MCC and the properties of fibrillated MCC are largely affected by the size and geometry of the functional groups of the silanes. After ball-milling, most MCC displayed enhanced e-beam tolerance and thermal stability, whereas the silane loading amount, surface area, and morphology of fibrillated MCC appeared to be random, which was exemplified by the proportional and non-proportional relationship between the loading amount and surface area of methyl silane- and phenyl silane-treated MCC, respectively. Density functional theory calculations and molecular dynamics simulations were employed to obtain the intricate details. The simulation results were in agreement with the experimental results. Finally, fibrillated MCC was incorporated into silicone foams as an additive. The thermal stability of fibrillated MCC with added silicone was greatly improved, and the tensile strength of fibrillated MCC-containing silicone foam was 44.1 and 5.4 times higher than that of the neat and MCC-containing silicone foams, respectively., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)