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Mental workload is a concept central to a range of disciplines (including cognitive psychology and ergonomics) that has given rise to various theoretical and methodological debates. As a result, researchers have used a number of techniques for measuring mental workload. Traditionally, three categories of measurement technique have been recognized: performance measures (e.g., the dual-task paradigm), subjective measures (e.g., rating scales), and physiological measures (e.g., heart, respiration, and blink rates). Each technique has advantages and limitations; however, some limitations may prevent an accurate evaluation of the mental workload. In this article, we focus on the benefits of combining multiple measures of mental workload. However, because combining several techniques is a very complex process, we have developed the Tholos software in an attempt to reduce this complexity. This software package uses measures from each of the three categories: a dual-task paradigm with auditory signals; the National Aeronautics and Space Administration task load index (NASA-TLX) scale and its simplified version, the "raw" task load index (RTLX); and physiological (such as pupil-dilation) measurements with which our software can merge results from the dual-task paradigm. To illustrate the benefits of using Tholos, we describe a puzzle-solving experiment in which we combined multiple measures of mental workload. The results indicate the importance of combining multiple measures to build upon the theoretical and methodological foundations of mental workload.