Molecular machine is one of the important fields in supramolecular chemistry. We are developing supramolecular systems exhibiting mechanical motions in the crystalline state. Since the molecules are anisotropically and densely arranged in the crystalline phase, molecular motions in a crystal can be easily extracted as an external output. Supramolecules are highly designable. A variety of combinations of inorganic or organic cations with crown ethers will exhibit diverse physical responses derived from dynamic feature of supramolecular systems. We have been combining the supramolecular cations with the anionic metal-coordination complex of [Ni(dmit)₂]^- (dmit^2- = 1,3-dithio-2-thione- 4,5-dithiolate^2-) showing peculiar magnetic and conducting properties due to the open-shell electronic structure. In this review, we introduce a series of multifunctional [Ni(dmit)2]^- supramolecular crystals exhibiting interplay between supramolecular motion and electronic functions.