A series of luminescent cyclometalated N<^>C<^>N [N<^>C<^>N = 1,3-bis(N-alkylbenzimidazol-2'-yl)benzene]platinum-(II) alkynyl and carbazolyl complexes has been prepared. The structure of one platinum(II) carbazolyl complex has been characterized by X-ray crystallography. The corresponding electro-chemical and photophysical properties have been explored and analyzed. The N<^>C<^>N platinum(II) complexes displayed, rich luminescence in degassed dichloromethane solution with their emission profiles dependent on the coordinated alkynyl and carbazolyl ligands. Their emission energies are correlated to the electronic properties of the alkynyl and carbazolyl ligands. By varying the electronic properties of the alkynyl and carbazolyl ligands, emission energies could be fine-tuned to cover a wide range of-the visible spectrum as supported by computational studies. A donor-acceptor platinum(II) complex has been utilized to fabricate memory devices that exhibit binary memory performances with low operating voltages, high ON/OFF ratios,, and long retention times. Solution-processable OLEDs have been fabricated based on another platinum(II) carbazolyl complex, resulting in a maximum external quantum efficiency of up to 7.2%, which is comparable to that of the vacuum-deposited devices based on the small-molecule counterpart, illustrating the multifunctional nature of the platinum(II)-containing materials.