To get a range of crystallite size, 5 N pure polycrystalline zinc specimens were shined with 50–100 Nd:YAG laser shots. Williamson-Hall, Size-Strain Plot, Halder-Wagner, and Wagner-Aqua models were employed to evaluate the crystallite size and lattice strain of pristine and laser-treated specimens. Surface hardness of the specimens were measured under 0.2 and 0.3 kgf indentation loads for 10 s. In each case, the surface hardness followed inverse Hall – Petch Relation. For a fixed number of laser shots, the surface hardness was greater for 0.2 kgf indentation load than that for 0.3 kgf. The surface hardness of pristine zinc specimen increased on treatment with 50 laser shots. With further rise in laser shots up to 80, the surface hardness progressively decreased close to that of pristine specimen. Later, it again increased for 90 laser shots and then slightly decreased for 100 laser shots.