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Background Since the start of the COVID‐19 pandemic, virtual reality simulation, including web‐based simulation, has increased in nursing education. This study explored nursing students' self‐directed problem‐solving in web‐based virtual simulation experiences. Method Convenience sampling yielded 16 Korean senior nursing students who had experienced clinical practice in the last semester. Data were collected from August 2020 to January 2021 through in‐depth Zoom video interviews and organized using NVivo version 12.0. Thematic analysis was applied to analyze the data. Results The following four themes were identified from nursing students' learning experiences during the web‐based virtual simulations: “self‐awareness of a lack of nursing competency in virtual reality,” “applying new learning strategies learned from failure,” “voluntary learning behavior,” and “cognitive shift toward a holistic understanding.” Web‐based virtual simulations activated various cognitive and metacognitive factors of self‐directed learning, and the system's prompt feedback and students' reflections facilitated learning effects. Nursing students corrected their cognitive errors while learning from their failures and mistakes and gained a holistic view of nursing practice. Conclusion In this study, web‐based self‐directed learning activated the metacognition of nursing students in a virtuous cycle. The virtual environment with no actual harm to the patient has become a space for learners to experience a sense of confidence, achievement, and satisfaction. Web‐based virtual simulation can be an effective teaching method to improve nursing students' self‐directed learning abilities and nursing competency.