Nonlinear-laser properties of crystals of non-centrosymmetric orthorhombic semi-organic tris(glycine) zinc chloride Gly 3 ·ZnCl 2 are reported in this paper. Under one-micron picosecond pumping many-phonon high-order SRS, a more than two-octaves Stokes and anti-Stokes lasing frequency comb, "Cherenkov"-type SHG, THG, and several cascaded parametric self-sum-frequency generation processes were observed. All recorded Raman-induced laser wavelengths were identified and attributed to the χ (3) -promoting vibration modes of the crystal. A brief review of nonlinear-laser properties of known SRS-active heterodesmic semi-organic crystals with partially ionic bonding character between structural units is given as well.Example of crystals of Gly3·ZnCl2 grown from aqueous solution