The new ionic intercalation compound (NH+4)0.22TiS0.22-2 has been synthesized by vacuum deintercalation of ammoniated TiS2, characterized by thermogravimetric analysis and powder X-ray diffraction, and examined by SQUID magnetometry (indirectly), differential scanning calorimetry, incoherent inelastic neutron scattering, and nuclear magnetic resonance. Although the diffraction pattern of this compound resembles a stage-II structure in which every other van der Waals gap is occupied by NH+4 it cannot be indexed completely on this basis. Magnetic and calorimetric measurements show that one electron is transferred to the host TiS2 conduction band per NH+4 cation and that the deintercalation enthalpy of NH+4 is 22 kcal/mol NH+4, respectively. Neutron scattering has provided evidence for an NH+4 torsional fundamental mode at 215 cm-1. The proton NMR linewidth and spin-lattice relaxation time are independent of temperature between 100 and 540 K, and the linewidth of 2.6 ± 0.3 G is in good agreement with that calculated for isotropic reorientation of the NH+4 cations.