X-ray crystallography and solid-state NMR techniques were used to determine the structure and Pt-195 NMR chemical shift ( CS) tensor of Pt[ S2C2( CF3)(2)](2). This is the first reported crystal structure of a highly oxidizing ( CN- or CF3-substituted) neutral bis( dithiolene) complex of a Ni triad metal in its pure form. The Pt-195 NMR CS tensor is highly anisotropic and asymmetric; the latter property is attributed to the noninnocent nature of the ligand. The tensor components and orientation are determined with density functional theory calculations.