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The 100% phase pure calcium silicate nanoparticles (CSNPs) of the α‐wollastonite phase by hydrothermal synthesis is achieved first. Next this work reports the first‐ever microwave‐assisted low temperature synthesis of calcium silicate‐cellulose nanograss composites. The characterization by FESEM studies confirm that calcium silicate‐cellulose composites possess the nanograss like morphology spread over the matrix of calcium silicate. The structural information of the calcium silicate‐cellulose composites are derived by both theoretical and experimental techniques. Low‐energy ground state geometrical structures of the cellulose on the triclinic wollastonite surfaces and their interactions have been primarily determined by Density Functional Theory. Accordingly, the short‐range structural information is confirmed by Pair Distribution Function analysis. Structural information along with binding interactions are also confirmed from X‐ray photoelectron spectroscopy. The implications of these detailed analysis of structures in tuning the properties of such ceramic polymeric hybrid composites for futuristic endodontic application is discussed. [ABSTRACT FROM AUTHOR]