In this article, core‐shell structured calcium copper titanate@polyaniline (CCTO@PANI) was synthesized using a simple procedure involving in situ polymerization of aniline in aqueous hydrochloric acid solution. Then, polydimethyl siloxane (PDMS) filled with self‐prepared CCTO@PANI particles had high dielectric constant, low dielectric loss, and actuated strain which was greatly improved at low electric field. Meanwhile, the elastic modulus of CCTO@PANI/PDMS composites was increased slightly only with a good flexibility. Compared to pure silicone elastomer (8.94%), the CCTO/PDMS and CCTO@PANI/PDMS (The weight ratio of CCTO and aniline was 10) composites exhibited a greater actuated strain of 10.95% and 13.24% at a low electric field and filling content of 10 V/μm, respectively. This study provided a simple and effective method for the improvement of actuated strain at low electric field through addition of CCTO@PANI/PDMS composites due to the hyper‐electronic polarization and a strong polaron delocalization, facilitating the wide application of dielectric materials. POLYM. COMPOS., 40:E62–E68, 2019. © 2017 Society of Plastics Engineers
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