Visible room-temperature photoluminescence (PL) was observed from hydrogen-free nanostructured amorphous carbon films deposited by pulsed laser ablation in different background pressures of argon (P_Ar). By varying P_Ar from 5 to 340 mTorr, the film morphology changed from smooth to rough and at the highest pressures, low-density filamentary growth was observed. Over the same pressure regime an increase in the ordering of sp² bonded C content was observed using visible Raman spectroscopy. The origin of the PL is discussed in terms of improved carrier localization within an increased sp² rich phase.