A survey of more than 1000 people by the Australia Institute found 83 per cent of respondents said supermarkets were responsible for a great deal or some of the blame for cost-of-living pressures.
More than four in five blamed energy companies, while 73 per cent said the onus was on banks and 71 per cent on the government.
When asked about the most visible source of rising prices, three in five people said groceries, followed by utilities at 21 per cent and transport at seven per cent.
The findings are considerably different to a recent Resolve Political Monitor poll, which found 36 per cent of respondents held governments most responsible for living costs.
Another 13 per cent blamed global factors outside Australia's control and the same number of people held businesses responsible.
Leah Heap, who co-wrote the Australia Institute report, said the message from consumers was loud and clear.
"Australians are pointing the finger at supermarkets as public enemy number one in the cost-of-living crisis," she said.
"It's clear Australia's supermarket duopoly is on the nose with the electorate."
A Woolworths spokeswoman said there were a range of factors behind rising costs.
"Many of the increased costs households are facing are also unfortunately making it more expensive for our suppliers to producers food and groceries - from electricity and fuel, to rent and interest rates," she said.
Coles was contacted for comment.
The two retail giants have for months been accused of ripping off suppliers, suffocating competitors and price-gouging customers.
The Australian Competition and Consumer Commission has taken Coles and Woolworths to the Federal Court, after accusing them of misleading discount pricing claims.
Anthony Albanese has gone after the two supermarkets for shrinkflation - when items decrease in size or quantity while the prices stay the same.
The Nationals have been pushing for the forced break-up of the giants, while Opposition Leader Peter Dutton has accused them of muscling out competition by keeping undeveloped land near their stores.
Almost two in three participants in the Australia Institute research said it was important to increase competition in the supermarket sector.
The same number of people said it was important to lower the cost of utilities to relieve cost-of-living pressures.
The survey comes as the federal government pledged $30 million for the consumer watchdog to investigate wrongdoing in the supermarket sector.
It found cost-of-living pressures were also impacting on people spending less on essential items.
More than a third of respondents spent less on heating or cooling in their home, two in five people shunned healthy food and 26 per cent cut back on GP visits.
"Addressing the cost-of-living crisis requires a multi-dimensional approach, rather than a singular reliance on high interest rates to slow inflation," Ms Heap said in the report.
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