In this study, the effect of zinc impurity on the organic high explosive pentaerythritol tetranitrate (PETN) single crystal has been investigated with optical microscopy and ex situ atomic force microscopy (AFM). The optical images show that the crystal shape has a transition with a predictable trend from long crystal to compact one as the zinc concentration is increased. Also, the 2-dimentional (2-D) growth hillocks are observed clearly on (110) face with contact AFM. The crystal growth occurs on monomolecular steps generated by 2-D nucleation and followed by layer-by-layer expansion, and the macro-steps formed onto the surface before spreading laterally as step bunches. The zinc ions are incorporated in growth steps as the zinc concentration is increased. The mechanism of inorganic impurity on molecular crystallization growth is still unclear. However, the incorporation of impurities may significantly affect growth kinetics of defect structure, and the bulk properties of molecular crystals.