Due to their portability, sensitivity, and ease of use, electrochemical sensors have recently become a popular method for rapid, on-site analysis. This study presents a proof of principle for the application of modified screen-printed carbon electrodes (SPCEs) for the detection of signature metals (Pb, Sb, and Zn) commonly found in gunshot residue (GSR), as well as for the detection of nitrate/nitrite in organic GSR and low explosives. To achieve these two aims, we have examined various electrode surface modifications. For metal detection, SPCEs were modified by electrodeposition of gold to improve sensitivity. GSR samples taken from two types of cartridge cases and shooting-related surfaces were analyzed using the Au-modified SPCEs. For nitrate/nitrite analysis, further electrode surface modifications were carried out by depositing Cu(II) onto the Au-SPCEs to enhance signal through catalytic activity of the copper surfaces. Both unburned and burned forms of black powder samples, as well as burned smokeless powder, were then analyzed using the Cu/Au-SPCEs. In conclusion, due to their low cost and portability, these sensors should prove useful for rapid forensic examination.