Abstract A new poly(dimethyl siloxane) (PDMS) composite was developed based on the 3D porous interconnected framework that is fabricated from reduced graphene oxide (rGO) and Dy 2 O 3 decorated single‐walled carbon nanotube (Dy 2 O 3 @SWNT). Despite merely containing ~0.6 wt% fillers, the composite prepared by backfilling 3D framework (3D‐Dy 2 O 3 @SWNT‐rGO) with PDMS prepolymer acquires as high as 32.9 dB of absorption‐dominated (92.3%–96.9%) electromagnetic interference (EMI) shielding effectiveness in X‐band, and up to 47% and 52% increments of respective compressive strength and modulus at 50% strain relative to PDMS. These performances result from the excellent combination of electrical conductivity (up to 0.317 S cm −1 ), magnetism (up to 7.1 × 10 −5 emu g −1 of susceptibility), and mechanical toughness (complete recovery after 80% compression) in a single three‐component filler system of 3D‐Dy 2 O 3 @SWNT‐rGO. Moreover, the organic integration of mechanical flexibility of PDMS with shape‐tunable ability of 3D‐Dy 2 O 3 @SWNT‐rGO enables PDMS composites developed here to EMI‐shield any shape surfaces.