Oil has been seeping into a nearby lake since the spring.
Now, the walkers want to bring attention to the 1.6 million litres of bitumen that was spilled.
A new report by the province also suggests groundwater in the area may also have been contaminated.
Participants in the ceremonial march told CBC's Laura Osman they want more action from the company and governments.
"I'd like to see the CNRL and all the oil companies stop what they're doing right now and clean up the oil that they spilled before they continue," said Nancy Scanie, an elder with the Cold Lake First Nation.
Scanie also said she would like Prime Minister Stephen Harper to pay more attention to the concerns of Canadians over the concerns of the oil industry.
"We cannot drink oil, and we sure in the world cannot eat the money. So we have to take care of our animals, our people, our children and our unforeseen children that aren't coming yet."
Along the way Saturday, walkers were chanting and playing horns as they walked along the highway, slowing traffic between Cold Lake and Bonnyville.
The walk will wrap up Monday evening as the group walks nearly 40 kilometres from Bonnyville back to the Cold Lake First Nation Dene Casino.
In total, the full “circle of solidarity” will be about 100 kilometres.
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