A novel multicomponent cascade cyclization and sulfenylation/selenation using aryl methyl ketones, isoquinolin-1-amine, and sodium arylsulfinates/1,2-diphenyldiselane to synthesize imidazo[2,1-a]isoquinoline derivatives in one-pot via the construction of two C-N bonds and one C-S/C-Se bond has been reported. This multicomponent reaction realizes simultaneous C(sp3)-H amination and sulfenylation/selenation, avoiding complicated prior substrate preparation. This process has simple operating conditions and good substrate compatibility.