Raman spectroscopic analysis of the pyrolyzed cellulose revealed further details on the formation of graphenic material (Fig. ). For superficially-pyrolyzed samples, the fluorescence signal from the cellulose paper dominates, but this disappears as the electrical resistance decreases. In addition, the peaks characterizing the sp 2 -hydridized carbon network (G band) and the finite lateral size of the graphitic crystallites (D band) (37) emerge at 1577±2 cm -1 and 1339±2 cm -1 , respectively. By increasing the laser power from 2.4 to 4.8 W, the ratio of D-band to G-band peak areas gradually decreases, indicating lateral growth of crystallite domains . Conversely, the 2D band at 2665±5 cm -1 , originated from the D-band overtone and sensitive to graphene stacking, becomes more prominent as laser power increases, evidencing the emergence of thin graphene domains. The multi-component and broadband nature of the 2D-overtone (Figs. and) further suggests a high degree of graphitization with turbostratic stacking between the graphenic layers . Notably, we did not observe significant shifts in peak positions upon growth of the crystallite domains (Fig. ). Early reports on the formation of laser-pyrolyzed conductive materials have relied exclusively on Raman spectroscopy . However, this approach provides a qualitative, or at best semi-quantitative, assessment of structural parameters. To gain quantitative insights into the evolution of their structural parameters, we carried out wide-angle X-ray scattering (WAXS) to correlate materials conductivity with graphenic crystallography. After isolating the pyrolyzed material, we were able to identify diffractograms of graphitic materials exhibiting the (002), and diffraction peaks (Figs. and). It should be noted that turbostratic layered materials have indistinguishable (101) and (100) peaks, and are thus assigned as here; the same applies to the (11) peak.