The 'Kiss You' hitmakers jetted out to the continent and began their week visiting local people in the deprived area of Accra, Ghana, for the British charity ahead of its Red Nose Day 2013 telethon, reported BBC online.
After spending time entertaining children in a school and raising donations for the poverty-stricken town, the boys - Niall Horan, Harry Styles, Liam Layne, Zayn Malik and Louis Tomlinson, described it as 'the best' and most 'amazing' experience they have ever had and have urged people to help the cause.
"Just arrived back from Accra, Ghana! Best experience ever! This red nose day please get involved," Horan posted.
Styles also shared his feelings about the trip, tweeting shortly after, "Today was the most amazing day I've had so far.. In my life ever."
The pop stars are believed to have headed over to Cape Town, South Africa, following their visit to Ghana to shoot a music video for the charity.
Comic Relief's Red Nose Day takes place on March 15 and includes various celebrities taking part to help transform the lives of countless people, both here at home in the UK and across Africa.