The mechanosynthesis route is a physical top–down strategy to produce different nanomaterials. Here, we report the formation of graphene nanoribbons (GNRs) through this route using carbon bars recovered from discarded alkaline batteries as raw material. The mechanosynthesis time (milling time) is shown to have an influence on different features of the GNRs such as their width and edges features. TEM revealed the presence of GNRs with widths of 15.26, 8.8, and 23.55 nm for the milling times of 6, 12, and 18 h, respectively. Additionally, the carbon bars evolved from poorly shaped GNRs for the shortest milling time (6 h) to well-shaped GNRs of oriented sheets forming for the longest milling time. Besides GNRs, graphene sheets (GNS) of different sizes were also observed. The Raman analysis of the 2D bands identified the GNS signal and confirmed the GNRs nature. ID/IG values of 0.21, 0.32, and 0.40 revealed the degree of disorder for each sample. The in-plane sp2 crystallite sizes ( La) of graphite decreased to 91, 60, and 48 nm with increasing peeling time. The RBLM band at 288 cm− 1 confirmed the formation of the GNRs. Mechanosynthesis is a complex process and the formation of the GNRs is discussed in terms of a mechanical exfoliation, formation of graphene sheets and its fragmentation to reach GNR-like shapes. It is shown that the synthesis of GNRs through the mechanosynthesis route, besides the use of recycled materials, is an alternative for obtaining self-sustaining materials.