With the recent interest in data storage in flexible electronics, highly reliable charge trap-type organic-based non-volatile memory (CT-ONVM) has attracted much attention. CT-ONVM should have a wide memory window, good endurance, and long-term retention characteristics, as well as mechanical flexibility. This paper proposed CT-ONVM devices consisting of band-engineered organic-inorganic hybrid films synthesized via an initiated chemical vapor deposition process. The synthesized poly(1,3,5-trimethyl-1,3,5,-trivinyl cyclotrisiloxane) and Al hybrid films are used as a tunneling dielectric layer and a blocking dielectric layer, respectively. For the charge trapping layer, different Hf, Zr, and Ti hybrids are examined, and their memory performances are systematically compared. The best combination of hybrid dielectric stacks showed a wide memory window of 6.77 V, good endurance of up to 10(4) cycles, and charge retention of up to 71% after 10(8) s even under the 2% strained condition. The CT-ONVM device using the hybrid dielectric stacks outperforms other organic-based charge trap memory devices and is even comparable in performance to conventional inorganic-based poly-silicon/oxide/nitride/oxide/silicon structures devices. The CT-ONVM using hybrid dielectrics can overcome the inherent low reliability and process complexity limitations of organic electronics and expedite the realization of wearable organic electronics.