A kind of silicone rubber (SR)/carbon fiber (CF)@polydopamine (PDA) flexible composites were prepared in this work. CF was modified by oxidative self‐polymerization of dopamine (DA), and the effect of DA concentration on properties of SR/CF@PDA composites was researched. The transverse fiber bundle tests have shown that SR/CF@PDA‐1.5 has the best interfacial bonding performance. Compared with SR/CF, tensile strength and elongation at break of SR/CF@PDA‐1.5 were increased by 61.7% and 68.4%, respectively. Results indicate that the interfacial bonding of SR/CF@PDA composites was effectively improved due to the adhesion properties of PDA. Moreover, the rough surface of CF@PDA also enhanced the interface interaction through physical “interlocking.” When being compared to other surface modification process, dopamine‐modified carbon fiber is cost effective, “green” and highly efficient. SR/CF@PDA with an excellent interfacial bonding and flexibility is a kind of wrapping material for protection of special precision instruments.
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