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The best way from Phuket may be bus.
Take a bus to Hat Yai from Phuket Town, maybe 300 baht or something.
When you arrive at Hat Yai, you can take another bus to either Kuala Lumpur, Penang or Singapore.
I am sure the buses may be more comfortable than the trains, airconditioned and with movies on TV screen.
I think you may be able to take train from Hat Yai to KL aswell but I am not sure.
I prefer airplanes thought, if you would like to skip bus the down to Hat Yai you can take airplane to Hat Yai for 1250 baht and then continue into Malaysia.
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