Some unique features of 1-isothiocyanatosilatrane, 1, include concomitant NMR couplings of quadrupolar N-14(NCS) nucleus with adjacent heteroatoms [J(C-13-N-14) = 26.17 Hz; J(Si-29-N-14) = 28.47 Hz] and the crystallographically determined shortest N-Si bond, 2.007(3) Angstrom, as well as a nearly linear structure of the heteroatoms N(1)-Si-N(2)-C(7)-S(1). Contrary to the known reactivity of tetracoordinate isothiocyanatosilanes, 1 invariably shows retention of the Si-N(CS) bond under normal nucleophilic/electrophilic reaction conditions. These novel features also get support from semiemperical MO calculations on the compound.