Thin-film microelectrode arrays have a wide variety of applications in research and medical devices. Conventionally, these arrays are fabricated through the use of photolithography, which can be problematic for innovative medical device fabrication due to long process times, inflexibility to design changes, and the reliance on potentially harmful chemicals. Here, we present the use of laser micromachining as an alternative to photolithography processes to fabricate thin-film polyimide microelectrode arrays. This fabrication method lends itself to an iterative design process as it can reduce fabrication steps and is attractive for medical devices since it can be used without harmful chemicals. Several process parameters were explored and the performance of the fabricated electrodes was compared to similar electrodes that were fabricated with conventional photolithography processes.