The objective of the present research work is to optimize the growth conditions of bi- tri- and few-layer graphene using pulsed laser deposition (PLD) technique. The graphene was grown on n-type silicon (1 0 0) at 530 °C. Raman spectroscopy of the grown films revealed that the growth of low defect tri-layer graphene depended upon Ni content and uniformity of the Ni film. The line profile analysis of the AFM micrographs of the films also confirmed the formation of bi- tri- and a few-layer graphene. The deposited uniform Ni film matrix and carbon/Ni thickness ratio are the controlling factors for the growth of bitri- or few- layer graphene using pulsed laser deposition technique.