The　development　of　new-type　memristors　with　special　performance　is　of　great　interest.　Herein,　an　inorganic-organic　hybrid　crystalline　polyoxometalate　(POM)　with　usual　dynamic　structures　is　reported　and　used　as　active　material　for　fabricating　memristor　with　unique　temperature-regulated　resistive　switching　behaviors.　The　hybrid　POM　not　only　exhibits　tunable　thermochromic　properties,　but　also　thermal-induced　reversible　aggregation　and　disaggregation　reactions,　leading　to　reversible　structural　transformations　in　SCSC　fashion.　Further,　the　memory　device　using　the　hybrid　POM　as　active　layer　exhibits　uncommon　performance,　which　can　keep　resistive　switching　silent　in　the　low　temperature　range　of　30–150　°C,　but　show　nonvolatile　memory　behavior　in　the　high　temperature　range　of　150–270　°C.　Particularly,　the　silent　and　working　states　at　three　special　temperatures　(30,　150　and　270　°C)　can　be　monitored　by　chromism.　The　correlation　between　structure　and　resistive　switching　property　of　the　material　has　been　discussed.　The　work　demonstrates　that　crystalline　inorganic-organic　hybrid　POMs　are　promising　materials　for　making　memristors　with　superior　performance.　©　2021　Wiley-VCH　GmbH