The　exploration　of　novel　photo/thermal-responsive　nonvolatile　memorizers　will　be　beneficial　for　energy-saving　memories.　Herein,　new　<110>-oriented　perovskites　using　single　template　melamine,　i.e.,　[(MLAI-H2)(PbX4)]n　(X　=　Br　(α-1),　Cl　(α-2),　MLAI　=　melamine)　have　been　prepared　and　their　structures　upon　irradiation　of　visible　light　have　been　investigated.　They　have　been　fabricated　as　nonvolatile　memory　devices　with　structures　of　ITO/[(MLAI-H2)(PbX4)]n/PMMA/Ag　(device-1:　X　=　Br,　device-2:　X　=　Cl),　which　can　exhibit　unique　visible　light-triggered　binary　nonvolatile　memory　performances.　Interestingly,　the　silent　or　working　status　can　be　monitored　by　visible　chromisms.　Furthermore,　the　light-triggered　binary　resistive　switching　mechanisms　of　these　ITO/[(MLAI-H2)(PbX4)]n/PMMA/Ag　memory　devices　have　been　clarified　in　terms　of　EPR,　fluorescence,　and　single-crystal　structural　analysis.　The　presence　of　light-activated　traps　in　<110>-oriented　[(MLAI-H2)(PbX4)]n　perovskites　are　dominated　in　the　appearance　of　light-triggered　resistive　switching　behaviors,　based　on　which　the　inverted　internal　electrical　fields　can　be　established.　According　to　the　structural　analysis,　the　more　distorted　PbX6　octahedra,　higher　corrugated　<110>-oriented　perovskite　sheets,　and　more　condensed　organic-inorganic　packing　in　Br-containing　perovskite　are　beneficial　for　the　stabilization　of　light-activated　traps,　which　lead　to　the　better　resistive　switching　behavior　of　device-1.　This　work　can　pave　a　new　avenue　for　the　establishment　of　novel　energy-saving　nonvolatile　memorizers　used　in　aerospace　or　military　industries.　©　2023