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A high-yield and straightforward method is proposed to obtain an electromagnetic interference (EMI) shielding film based on multilayered Ti 3 C 2 T x (m-Ti 3 C 2 T x). Holocellulose nanofibrils modified by sulfamic acid (SHCNF) with unique "core-shell" structure can act as a dispersant and a binder to assist in exfoliating m-Ti 3 C 2 T x into delaminated-Ti 3 C 2 T x (d-Ti 3 C 2 T x) and fabricate flexible Ti 3 C 2 T x /SHCNF composite films with a high-yield value. The "brick-and-mortar" composite films exhibit a superior electromagnetic interference (EMI) shielding effectiveness (SE) of 45.02 dB with an ultrathin thickness of 40 μm at the 12.4 GHz. Moreover, these flexible and strong integrated Ti 3 C 2 T x /SHCNF composite films also display excellent specific EMI SE of SSE/t (4437 dB cm2 g−1) and high EMI shielding efficiency (99.996%). Therefore, the SHCNF-assisted method provides a cost-effective approach to fabricate a strong and flexible MXene-based nanocomposite films toward EMI shielding application. [Display omitted] • Holocellulose nanofibrils assisted in exfoliating multilayered Ti 3 C 2 T x. • The Ti 3 C 2 T x /SHCNF film exhibited superior mechanical properties. • The film presented excellent specific EMI shielding efficiency. [ABSTRACT FROM AUTHOR]