After complaining about chest pains on Monday, Shahjahan Bhuiyan, 74, was taken to the hospital in the country's capital, Dhaka. He later died while undergoing treatment, according to local media.
Bhuiyan is believed to have carried out at least 26 executions, with some sources putting the figure as high as 60.
As a former revolutionary, he became a hangman while serving a robbery and murder sentence for 42 years.
Bhuiyan's ambition to shorten his prison sentence by volunteering as an executioner was rewarded last year when he was released ten years early.
Among those who died at his hands were military officers convicted of murdering the country's founding leader, Sheikh Mujibur Rahman, the father of Bangladesh's current prime minister.
He also executed politicians Ali Ahsan Mujahid and Salahuddin Quader Chowdhury, both accused of war crimes, as well as serial killer Ershad Shikder.
Bhuiyan has always defended his duty as a hangman, claiming, "If I didn't hang them, someone else would."
A book detailing his experiences, including an explanation of the hanging method, was published earlier this year and received nationwide attention.
Bangladesh: Shahjahan Bhuiyan who hanged most notorious serial killers, dies at the age of 74
