Firearm related violence is a cause for concern in an ever-turbulent world. In this thesis, innovative electrochemical approaches to forensic evaluation of firearm generated evidence is presented using a two-prong approach. Firstly, development of an electroanalytical method for the detection of characteristic compounds found within the organic fraction of firearms residue (OFAR) was explored. This involved electrochemical analysis of diphenylamine (DPA) and ethyl centralite (EC) in both organic and aqueous supporting electrolytes revealing the formation of secondary products at the electrodes surface such as diphenylurea and primary amine degradation products. A novel sensing approach followed with the aid of magnetic nanoparticles of magnetite (MNPs) formed using controlled electrooxidation and chemical co-precipitation processes. Quantitative analysis using differential pulse voltammetry (DPV) revealed limits of detection (LODs) and quantification (LOQs) for EC and DPA at 4.39 ± 0.28 and 14.6 ± 0.95 μM and 3.51 ± 0.15 and 11.7 ± 0.47 μM respectively with sensitivities of 0.0637 ± 0.0044 and 0.0801 ± 0.0034 μA.μM-1. The method was applied to unburnt ammunition and real FAR samples while data from custom-designed screen-printed electrodes (SPE) highlighted the feasibility of onsite OFAR determination. Secondly, the deposition of conducting/redox active polymers for visualising latent finger-marks on brass ammunition casings was explored. This aspect exploited the electrodeposition of 3,4-ethylenedioxythiophene (EDOT), thionine Acetate (Th), neutral red (NR), and their mixtures at a range of transducers including sheet and cartridge brass. EDOT-Th emerged consistently as the most effective combination, revealing latent finger-marks at the highest level of detail (level 3), including pores within the ridges, on brass sheets using a rapid (120 s) and low-potential (0.1 V) approach. Successful visualisation of groomed latent finger-marks was achieved following exposure to temperatures of 700 °C and up to 16-month room temperature aging, with evidence for a robust methodology suitable for forensic practice. Bespoke electrochemical cells designed to facilitate the use of ammunition casings as working electrodes produced exceptional results via CV, resulting in pristine visualised latent finger-marks of grade 4 with visible level 3 features. Overall, the research advances the state of the art with respect to electroanalytical tools for OFAR measurement of signature analytes with the potential for extension to multiplexed operation.