The reduction of greenhouse gas emissions and the effort of carbon neutrality require the improvement of spark-ignition engines in terms of efficiency and capability to operate on renewable fuels. The electrode wear of spark plugs, used for ignition of novel fuels and lean mixtures, emerges as a significant challenge in this transition. Understanding the physical mechanism and influence of spark operation parameters of the wear process is thus important. Compared to the conventional methodology of performing long-term wear tests, laser-based optical diagnostics methods are capable of assessing electrode wear during one single or a few spark discharges. In this work, the necessary initial steps required for performing optical investigations using laser-induced fluorescence (LIF) are presented. Several excitation pathways of nickel atoms were investigated, and 336.96 nm was identified as the optimal one. This excitation approach yielded emissions between 338.75 and 353.58 nm, effectively avoiding the major interference from N