The development of a nanostructured copper–laser-induced graphene (LIG) composite that can catalyze the reduction of nitrate is described. The system was characterized using a range of surface analytical methods (SEM, Raman, DekTak profilometry). The electrochemical performance of the copper mesh in reducing nitrate was investigated, the nature of the catalytic response was elucidated, and the influence of potential interferences was critically appraised. The adaptation of the system as the basis of an electrochemical sensor for nitrate was assessed, which displayed a limit of detection of 4.7 μM nitrate. The analytical applicability in authentic media was evaluated through the analysis of two surface water samples and validated by standard spectroscopic (nitrate reductase–Griess methods). The LIG substrate offers a simple, scalable route towards the reduction of nitrate with a construction simplicity and sensitivity that is competitive with much more complex nanomaterials.