• A highly aligned and compact MXene film fabricated by continuous centrifugal spraying achieves ultra-broadband EMI shielding from GHz to THz bands.
• The film exhibits record-high specific shielding effectiveness of 1.545 × 10^6 dB cm2 g−1, surpassing previously reported shielding films.
• Ultra-low infrared emissivity (0.1) in the 2.5–16.0 μm range enables effective infrared stealth for day/night applications.
• Efficient electrothermal performance (saturated temperature >120 °C at 1.0 V, heating rate 4.4 °C s−1) offers multifunctional protection.