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• CBRSi is designed and synthesized through alkyne insertion, oxidation and esterification reactions. • CBRSi-CP is obtained via coupling and polycondensation reaction. • CBRSi-CP is transparant, flexible , superhydrophobic, and thermally stable. Cellulose Nanopaper is a kind of green material prepared from renewable cellulose nanofibrils. In order to achieve multi-functionization of cellulose nanopaper, thermally stable o-carborane moieties were introduced and grafted on the surface of cellulose nanopaper through silane coupling process. Firstly, o-carboranyl silane was designed and synthesized through alkyne insertion, oxidation and esterification reactions. Then o-carboranyl silane modified cellulose nanopaper was prepared via in-situ coupling and polycondensation reaction between o-carboranyl silane and cellulose nanopaper. The obtained nanopaper shows superhydrophobicity together with good transparency and flexibility. Besides, it exhibits improved dimensional stability and thermal stability owing to the introduction of o-carborane moiety. [ABSTRACT FROM AUTHOR]