Abstract Functional gradient films have attracted extensive attention due to the gradient changes in their microstructures. However, such well‐precise gradient structural control is still a critical challenge. Herein, with graphene oxide (GO) and single walled carbon nanotubes (SWNTs) as building blocks, a dynamical centrifugal casting strategy is proposed for the first time to construct supercontinuous gradient nanocarbon film (SGNF), in which gradient pore structure and electrical conductivity can be readily regulated by altering the reduction degree of GO. The as‐fabricated SGNF delivers an exceptional electromagnetic interference (EMI) shielding efficiency (SE) of 62 dB with an ultralow R (0.7), which can be further elevated to 98 dB after graphitization, reflecting an advantageous feature of adjustable absorption and high‐efficiency EMI SE. Moreover, the resulting SGNF exhibits satisfactory electrothermal performance in practical applications. This work offers a viable strategy for architecting supercontinuous gradient nanocarbon films with attractive performance advantages.