CHATGPT artificial intelligence is taking the world by storm, and countless electronic devices will generate massive amounts of electromagnetic interference (EMI). Hence, there is a pressing demand for materials exhibiting high thermal conductivity and superior EMI shielding effectiveness (SE). Thus, we construct a polyimide/carbon nanotube@Ag@polyimide/graphene (PCAPG) composite aerogel with porous, layered, and homogeneous structures in one, which provides a new idea for the multi-interface polarization interaction and special structure of anti-EMI materials. PCAPG has high thermal conductivity of ∼ 0.259 W (mK)-1 at 25 °C, excellent EMI SE of ∼ 90.28 dB and specific shielding effectiveness (SSE) of ∼ 940.42 dB cm3 g−1. The synergistic EMI attenuation mechanism of the PCAPG composite structure is analyzed using an aerogel unit. This composite aerogel provides a viable solution for infrared stealth, promoting heat dissipation from electronic components and reducing electromagnetic interference.