Materials based on transition metals, such as Cu, Co, and Ni, have been intensively used as electrocatalysts for non-enzymatic electrochemical glucose sensing. However, the current trend of wearable/in vivo continuous glucose sensing has raised the need for non/low-toxic candidates. Herein, we demonstrate that the overlooked low-toxic bismuth (Bi)-based nanomaterials are suitable choices. Using a laser-ablation method, surfactant-free Bi nanoparticles (NPs) and transition metal (Ni and Co)-doped Bi NPs are obtained, achieving amperometric sensitivity values of 127, 677, and 2326 µA mM−1 cm−2, respectively. Low detection limits of 1 and 4 µM, as well as an extensive linear range of 0.001–3.5 mM, are recorded using Ni- and Co-doped Bi NPs, respectively. With competitive performance and high selectivity towards glucose sensing in both standard and serum samples, Bi-based nanomaterials are proven effective and promising candidates for future glucose sensor design beyond transition metal elements.