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We travelled from Phuket to Krabi by private taxi (about 3 or 4 hours) and then once in Krabi we bought a "guided tour" ticket to Samui. This was an all-day trip that started on a minivan, then on a big bus, then the ferry ride to Samui and then another mini van to take us to our hotel. This took all day. Depending on how long you are visiting Thailand, I wouldn't recommend this route if you are on a short holiday.
We flew back to Phuket from Samui in about 2 hours compared to our day and a half adventure going the other way. Although it was pretty cool to see some of the landscape of Thailand that we wouldn't have otherwise seen.
So, if you aren't able to get a flight to Samui, it is possible, but very lengthy.
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