Archaeologically, Kalambo Falls is one of the most important sites in Africa. It has produced a sequence of past human activity stretching over more than two hundred and fifty thousand years. It was first excavated in 1953 by John Desmond Clark who recognised archaeological activity around a small basin lake behind the falls.
Late Acheulian stone tools, hearths and well preserved organic objects were found there including a wooden club and digging sticks and evidence of fruit consumption. Tools excavated from Kalambo Gorge have been radiocarbon-dated to be from around 300 000 BC, and the hearths indicate people were using fire systematically there some 60 000 years ago.
The Acheulian industry was superseded by the Sangoan and then Lupemban industries related to those found in the Congo. Around 10,000 years ago the site was occupied by the Magosian culture which in turn gave way to Wilton activity. Finally, around the fourth century AD, a more industrialised Bantu people began to farm and occupy the area.
In 1964 the archaeological site was gazetted as a national monument by Zambia's National Heritage Conservation Commission.
The falls' cliff-face ledges provide nesting places and breeding sites for a Marabou Stork colony.