The films of few-layer graphene are formed through laser exfoliation of a highly ordered pyrolytic graphite (HOPG), without a catalytic layer for the growth process. The femtosecond (fs) laser exfoliation process is investigated at different laser fluences and substrate temperature. For fs laser exfoliation of HOPG, the few-layer graphene is obtained at 473 K under an optimal laser fluence. The formation of few-layer graphene is explained by removal of intact graphite sheets occurred by an optimal laser fluence ablation. The new insights may facilitate the controllable synthesis of large area few-layer graphene.