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A series of BT–cCNT/PDMS and BT–aCNT/PDMS composites were developed by incorporating barium titanate (BT) nanoparticles together with carboxylic functionalized multiwalled carbon nanotubes (cCNT) and amino functionalization multiwalled carbon nanotubes (aCNT) in polydimethylsiloxane (PDMS). Benefitting from the abundant active groups, CNTs and BTs can be in situ “bridged” by hydrogen bond in all of the BT–cCNT/PDMS and BT–aCNT/PDMS composites. Here, we studied the effect of hydrogen bonds (type and amount) between BTs and CNTs at the interface and dielectric properties of the composites. The results indicated that the BT–cCNT/PDMS composite exhibited higher dielectric constant and comparable dielectric loss than the BT–aCNT/PDMS composite, especially when weightCNT < 1 wt%. Also, the dielectric properties of BT–cCNT/PDMS composite show stronger temperature dependence than BT–aCNT/PDMS composite. Finally, the tailorable performance of the polymer‐based dielectric composites can be obtained by regulating the interface with the help of hydrogen bonds.

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Recently, polydimethylsiloxane (PDMS)-based porous materials have been regarded as ideal candidates in various applications. We created a PDMS composite sponge decorated with reduced graphene oxide (rGO)/carbon nanotube (CNT) fillers via polydopamine (PDA). Specifically, a manufactured PDMS sponge was prepared by a sacrificial template approach and then PDA was decorated on a network of PDMS sponges by dopamine selfpolymerization. PDA tightly and firmly attached to the PDMS sponge skeleton, which makes the superhydrophobic PDMS sponge hydrophilic providing adsorption sites for rGO and CNT fillers; thus, the compatibility between fillers and the PDMS matrix was improved. The developed rGO-CNT/PDA@PDMS composite sponge exhibited excellent sensing characteristics, photothermal effect, and superwettability simultaneously. The rGO-CNT/PDA@PDMS-based sensor has a wide strain range (0−60%), high sensitivity (GF = 2.13), and stability (500 loading/unloading cycles). Additionally, rGO-CNT/PDA@PDMS exhibits excellent oil−water separation performance and high-efficiency absorption of oils. Simultaneously, the rGO-CNT/PDA@PDMS sponge was also proved to possess good photothermal conversion performance. Therefore, the environmentally friendly and multifunctional rGO-CNT/PDA@PDMS composite sponge exhibits superior potential for application in flexible intelligent wearable devices, oily wastewater, and seawater desalination.