A　novel　organosoluble　polyimide　(PI)　with　pyrimidine　ring　in　the　main　chain　was　synthesized　by　chemical　and　thermal　imidization,　respectively,　from　3,3,4,4-benzophenone　tetracarboxylic　dianhydride　and　2,4-diamino-6-chloropyrimidine　as　raw　materials　and　its　molecular　structure,　solubility,　UV-visible　absorption　characteristic,　crystallinity,　thermal　stability,　electrochemical　behaviors,　and　mechanical　properties　were　also　studied.　It　was　found　that　the　introduction　of　pyrimidine　ring　in　the　main　chain　could　increase　the　solubility　of　PI　in　polar　aprotic　solvents　at　room　temperature　and　60　degrees　C,　respectively,　because　of　its　molecular　main　chain　with　asymmetric　structure　and　two　polar　N　atoms　in　pyrimidine　ring.　Furthermore,　PI　had　strong　optical　absorption　peak　intensity,　excellent　thermal　stability,　good　redox　reversibility,　especially　outstanding　mechanical　properties,　which　were　conductive　to　its　potential　applications　in　adhesives,　polyelectrolyte,　separation　membrane,　and　so　on.　(c)　2016　Wiley　Periodicals,　Inc.　J.　Appl.　Polym.　Sci.　2016,　133,　43680.