Abstract A new strategy for multilayer stacking using charge trapping layer (CTL) is proposed and a new CTL material is synthesized, which contains a trilayer dielectric with the total thickness less than 28 nm, deposited by initiated chemical vapor deposition (iCVD) process. 2.6 nm thick poly(1,3,5‐trimethyl‐1,3,5‐trivinyl cyclotrisiloxane) (pV3D3) and 19 nm thick poly(1,4‐butanediol diacrylate) (pBDDA) are employed as tunneling and blocking dielectric layers, respectively. A 6 nm thick ultrathin charge trapping layer containing hydroxyl group is inserted between the tunneling and the blocking layers for stable, long‐term memory operation. For this purpose, a homogeneous copolymer of 1,4‐butanediol diacrylate and 2‐hydroxyethyl acrylate is newly synthesized. The fabricated memory with the trilayer dielectric shows larger than 5.8 V of memory window at low programming/erasing voltage of 16 V. The retention characteristics of the low‐power organic memory device is improved significantly with the drain current decrease less than 0.40 order after 10 8 s, corresponding to one of the longest retention time periods obtained from organic NVM reported to date. The low‐power organic NVM could also be integrated on flexible substrate, which is fully operational even under 2.72% of applied strain.