Chanderpaul, 31, was given the captaincy during the contracts row between leading players and the West Indies Cricket Board (WICB) before the start of the South African series.
He informed the WICB of his decision on Tuesday and said: "I would like to take this opportunity to tender my resignation as captain with immediate effect.
"This would give me an opportunity to focus on my batting and other areas of my cricket where I would be able to make a more significant contribution to the team, by being more focused on my batting." Chanderpaul averaged 47 as captain, but struggled in the last eight months, scoring just 198 from 13 innings.
"I have served my time as the captain and would like to pass the mantle on to another person. I would fully support my replacement, and work towards the good of the team," he said. "I would like to thank all who worked with me during my tenure as captain, and I am looking forward to continuing my hard work for West Indies cricket."
Ken Gordon, the WICB president, emphasised Chanderpaul's importance to the team and denied that he was forced to resign. "No, I received Mr Chanderpaul's letter today," Gordon told CCN TV6. "In it he expressed his desire to focus more heavily on his batting...so I think it was a reasonable approach by him and I called him to thank him for it [his contribution] and to indicate to him that we are all very supportive of him."
Chanderpaul's last series as captain resulted in a 2-0 defeat to New Zealand. He leaves just a couple of weeks before the home international season begins with a one-day series against Zimbabwe, before the visit of India. The WICB have said a new captain will be named in the shortly.