The development of functional metalladithiolene complexes was described. Photo-, magneto-, and electro-functional moieties were hybridized with a metalladithiolene backbone to produce novel electronic properties, such as photo-controlled three-state switching, and a SOMO-HOMO converted electronic structure. Long range electronic communication and three-dimensional clusterization were achieved on triangular trinuclear metalladithiolene complexes. The atomiclayer nickel dithiolene nanosheet was successfully prepared, in which nickel bis(dithiolene)moieties were connected through benzene skeletons to form a fully π-conjugated hexagonal structure in two dimensions. The electric properties of the stacked nanosheets were modulated by chemical redox reaction.