Leo is to preside on Thursday over a peace meeting involving a Mankon traditional chief, a Presbyterian moderator, an imam and a Catholic nun.
The aim is to highlight the interfaith movement that has been seeking to end the conflict and care for its many traumatised victims.
The Pope is also set to celebrate a mass for the people of Bamenda, near Cameroon's western border with Nigeria.
Leo arrived in Cameroon on Wednesday on the second leg of his four-nation African trip, the first by the first American pope.
In his arrival speech, he demanded the "chains of corruption" in the mineral-rich country be broken and lectured President Paul Biya on the legitimate exercise of authority.
The 93-year-old Biya, the world's oldest leader, has been in power since 1982 and claims to have won a disputed election in 2025 that gave him an eighth term in office.
The conflict in Cameroon's two Anglophone regions is rooted in Cameroon's colonial history, when the country was divided between France and Britain after World War I.
English-speaking regions later joined French Cameroon in a 1961 UN-backed vote, but separatists say they have since been politically and economically marginalised.
In 2017, English-speaking separatists launched a rebellion with the stated goal of breaking away from the French-speaking majority and establishing an independent state.
The conflict has killed more than 6000 people and displaced over 600,000 others, according to the International Crisis Group.
On the eve of Leo's arrival, separatist fighters announced a three-day pause in fighting.
A spokesperson for the Unity Alliance, Lucas Asu, said the pause "reflects a deliberate commitment to responsibility, restraint and respect for human dignity, even in the context of ongoing conflict".
He said the Pope's visit should remain "spiritual" and not be seen as endorsing any political authority.
Though the number of deadly attacks by separatists has decreased in recent years, the conflict shows no sign of resolution.
Peace talks with international mediators have stalled, with both sides accusing each other of acting in bad faith.