Covalent　organic　polymer　(COP)　thin　film-based　memristors　have　generated　intensive　research　interest,　but　the　studies　are　still　in　their　infancy.　Herein,　by　controlling　the　content　of　hydroxyl　groups　in　the　aldehyde　monomer,　Py-COP　thin　films　with　different　electronic　push-pull　effects　were　fabricated　bearing　distinct　memory　performances,　where　the　films　were　prepared　by　the　solid-liquid　interface　method　on　the　ITO　substrates　and　further　fabricated　as　memory　devices　with　ITO/Py-COPs/Ag　architectures.　The　Py-COP-1-based　memory　device　only　exhibited　binary　memory　behavior　with　an　ON/OFF　ratio　of　1:101.87.　In　contrast,　the　device　based　on　Py-COP-2　demonstrated　ternary　memory　behavior　with　an　ON/OFF　ratio　of　1:100.6:103.1　and　a　ternary　yield　of　55%.　The　ternary　memory　mechanism　of　the　ITO/Py-COP-2/Ag　memory　device　is　most　likely　due　to　the　combination　of　the　trapping　of　charge　carriers　and　conductive　filaments.　Interestingly,　the　Py-COPs-based　devices　can　successfully　emulate　the　synaptic　potentiation/depression　behavior,　clarifying　the　programmability　of　these　devices　in　neuromorphic　systems.　These　results　suggest　that　the　electronic　properties　of　COPs　can　be　precisely　tuned　at　the　molecular　level,　which　provides　a　promising　route　for　designing　multi-level　memory　devices.　©　2024