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According to the transcripts of the mission, he turned the Lunar Module's engine off. He radioed Houston to let them & the world know that they had landed safely. He & Buzz Aldrin immediately prepared the Lunar Module ascent module to be ready to lift off again, in case of an emergency. Those were some of the first things he did. If you mean when he left the Lunar Module and WALKED on the surface, he took an emergency Moon soil/rock sample, in case they needed to leave the surface in an emergency, at least he brought back SOME lunar samples.

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Q: What was the first thing Neil Armstrong did on the surface of the moon?
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