"South Africa needs an honest, trustworthy and highly skilled leader, someone who can restore to our people hope and belief in our country," a Cope statement released on Friday said.
"We need a leader we can look up to and respect, a leader who can inspire South Africans to take our nation from being a good one to a great one."
Threat to ANC
Dandala, 57, helped mediate an end to violence as apartheid-era South Africa gave way to democratic rule.
His nomination by Cope could prove popular with South Africans who are unhappy with the ANC's record on fighting crime, corruption and healthcare.
Given that many of Cope's members are former ANC loyalists, the ruling party could lose its two-thirds majority in parliament, thus ending its ability to pass changes to the constitution.
Cope was established by former ANC officials unhappy with the party's decision to push Thabo Mbeki, Zuma's main rival, out of the presidency.
The new party had been led by Mosiuoa Lekota, a former defence minister, and Mbhazima Shilowa, the ANC's deputy party president.