The remarkable properties of carbon nanotubes (CNTs) have led to promising applications in the field of electromagnetic interference (EMI) shielding. However, for macroscopic CNT assemblies, such as CNT film, achieving high electrical and mechanical properties remains challenging, which heavily depends on the tube–tube interactions of CNTs. Herein, we develop a novel strategy based on metal–organic decomposition (MOD) to fabricate a flexible silver–carbon nanotube (Ag–CNT) film. The Ag particles are introduced in situ into the CNT film through annealing of MOD, leading to enhanced tube–tube interactions. As a result, the electrical conductivity of Ag–CNT film is up to 6.82 × 10⁵ S m⁻¹, and the EMI shielding effectiveness of Ag–CNT film with a thickness of ~ 7.8 μm exceeds 66 dB in the ultra-broad frequency range (3–40 GHz). The tensile strength and Young’s modulus of Ag–CNT film increase from 30.09 ± 3.14 to 76.06 ± 6.20 MPa (~ 253%) and from 1.12 ± 0.33 to 8.90 ± 0.97 GPa (~ 795%), respectively. Moreover, the Ag–CNT film exhibits excellent near-field shielding performance, which can effectively block wireless transmission. This innovative approach provides an effective route to further apply macroscopic CNT assemblies to future portable and wearable electronic devices.

碳纳米管（CNT）的卓越性能使其在电磁干扰（EMI）屏蔽领域具有广阔的应用前景。然而，对于宏观碳纳米管组件，例如碳纳米管薄膜，实现高电气和机械性能仍然具有挑战性，这在很大程度上取决于碳纳米管的管与管之间的相互作用。在此，我们开发了一种基于金属有机分解（MOD）的新策略来制造柔性银碳纳米管（Ag-CNT）薄膜。通过 MOD 退火，Ag 颗粒被原位引入 CNT 薄膜中，从而增强管与管之间的相互作用。结果，Ag-CNT薄膜的电导率高达6.82×10 5 ^S  m ^-1，厚度约7.8 μm的Ag-CNT薄膜的EMI屏蔽效能在超宽频率下超过66 dB范围（3–40 GHz）。Ag-CNT薄膜的拉伸强度和杨氏模量分别从30.09±3.14增加到76.06±6.20MPa(~253%)和从1.12±0.33增加到8.90±0.97GPa(~795%)。此外，Ag-CNT薄膜表现出优异的近场屏蔽性能，可以有效阻挡无线传输。这种创新方法为进一步将宏观碳纳米管组件应用于未来的便携式和可穿戴电子设备提供了有效途径。