Reported　herein　is　the　first　example　of　electrochemical　selenocyanation　of　imidazo[1,5-a]quinolines　with　KSeCN　under　metal　catalyst-　and　chemical　oxidant-free　conditions.　This　sustainable　strategy　shows　a　broad　scope　and　great　compatibility　with　functional　groups,　and　affords　synthetically　and　biologically　important　selenocyanated　imidazo[1,5-a]quinolines　in　good　to　excellent　yields　with　cheap　graphite　and　Ni　plates　as　the　electrodes.　The　gram-scale　synthesis　was　also　successfully　conducted,　which　might　demonstrate　the　potential　value　of　this　electrochemical　protocol.　(c)　2019　Chinese　Chemical　Society　and　Institute　of　Materia　Medica,　Chinese　Academy　of　Medical　Sciences.　Published　by　Elsevier　B.V.　All　rights　reserved.