In this work, few-layer graphene materials were produced from Fe-lignin nanocomposites through a molecular cracking and welding (MCW) method. MCW process is a low-cost, scalable technique to fabricate few-layer graphene materials. It involves preparing metal (M)-lignin nanocomposites from kraft lignin and a transition metal catalyst, pretreating the M-lignin composites, and forming of the graphene-encapsulated metal structures by catalytic graphitization the M-lignin composites. Then, these graphene-encapsulated metal structures are opened by the molecule cracking reagents. The graphene shells are peeled off the metal core and simultaneously welded and reconstructed to graphene materials under a selected welding reagent. The critical parameters, including heating temperature, heating time, and particle sizes of the Fe-lignin composites, have been explored to understand the graphene formation mechanism and to obtain the optimized process parameters to improve the yield and selectivity of graphene materials.