Organothiocyanate and organoselenocyanate compounds are of paramount importance in organic chemistry as they are key intermediates to access sulfur‐ and selenium‐containing compounds. Therefore, among the different synthetic pathways to get SCN‐ and SeCN‐containing molecules, original methodologies using electrophilic reagents have recently been explored. This Minireview will showcase the recent advances that have been made. In particular, the design of several electrophilic sources and their applications for the thiocyanation and the selenocyanation of various classes of compounds will be highlighted and discussed.