The linear and second-order nonlinear optical properties of single-crystal zinc tris(thiourea) sulfate, or ZTS, are determined. The deduced nonlinear coefficients are \d3l\ = 0.3l, \d32\ = 0.35, and \d33\ = 0.23 Pm/V compared with a \d14\ value of 0.39 pm/V for potassium dihydrogen phosphate. Because it exhibits a low angular sensitivity (delta-DELTA-k/delta-theta), ZTS may prove useful for type-II second-harmonic generation from 1.06 to 1.027-mu-m. We present the phase-matching measurement data for ZTS and compare the calculated frequency conversion efficiency for ZTS with that of several other well-characterized materials.