This case study focuses on a series of studies conducted by an Australian Psychology PhD candidate. The studies centered on an attempt to develop a novel method for decomposing expert decision processes among criminal investigators. The work built on previous research efforts that had a substantial emphasis on qualitative techniques (e.g., Cognitive Task Analysis) by “validating” resultant qualitative descriptions via a new computerized measure, which sought to quantify aspects of expertise. The project was somewhat unique in that it had both a basic emphasis (e.g., eliciting descriptions of cognitive processes) and an applied flavor (i.e., conducted in the field, with some immediate applications in mind). Data were collected from some of the most renowned law enforcement agencies on the planet (e.g., the Federal Bureau of Investigation, the Royal Canadian Mounted Police) and spread across multiple countries (e.g., Australia, the United States, and Canada). Testing was completed in a round-trip whereby qualitative data were transcribed, reduced to thematic descriptions, and coded for agreement during the first leg, whereas quantitative data were collected on the return, incorporating the thematic descriptions as stimuli in the computer task. The case study details numerous practical lessons of relevance to early career researchers, including the importance of preparation and ethical awareness, and the challenges associated with recruiting special samples and testing in the “noise” of naturalistic settings. Ultimately, the piece underlines the importance of being open to a range of research tools, which can be used in harmony to triangulate toward quality evidence while also emphasizing the vulnerability of exploratory and field-based research.