Present investigation is aimed to explore the single crystal growth, microhardness and third order nonlinear optical (TONLO) properties of Nd3+ doped zinc tris-thiourea sulphate (ZTS) crystal. The commercial slow solvent evaporation technique has been chosen to grow a good quality ZTS (12 mm × 0.5 mm × 0.3 mm) and Nd3+ doped ZTS (11 mm × 0.6 mm × 0.4 mm) single crystals. Vickers microhardness test has been employed to analyze the influence of Nd3+ dopant on the hardness behavior of ZTS single crystal. The TONLO effects occurring in Nd3+ doped ZTS single crystal have been evaluated by means of Z-scan technique using a He–Ne laser operating at 632.8 nm. The close and open aperture Z-scan configuration have been used to determine the nature of TONLO refraction n2 and absorption β, respectively. The magnitudes of vital TONLO parameters, such as refraction n2, absorption coefficient β, figure of merit and susceptibility χ3 of the Nd3+ doped ZTS single crystal, have been determined using Z-scan transmittance data. The n2, β, and χ3 of Nd3+ doped ZTS single crystal were found to be of the order of 10−10 cm2/W, 10−6cm/W and 10−5 esu, respectively.