Teamwork, communication, and workload issues continue to contribute to patient safety events. The authors developed a diagnostic mixed methods toolkit combining a behavior observation tool, semistructured interview guide, and surveys to proactively identify relevant gaps. Applied across 14 units at three hospitals, this toolkit yielded 344 findings with 156 associated recommendations and took, on average, four days of observation. On a scale from 1 (not at all helpful) to 6 (substantially helpful), leaders indicated that the assessment and its recommendations were very helpful (median 5, interquartile range 5-6, 34 survey respondents, 47.9% individual-level response rate, 85.7% unit-level response rate). Integrating this tool into a broader safety strategy can help inform organizational improvement efforts.