Dr Alan Billings, South Yorkshire's PCC, made his comments after two coroners raised concerns about deaths on a stretch of the M1 in the county.
Meanwhile, South Yorkshire Police has said it will examine inquest documents relating to two smart motorway deaths.
Highways England said it wanted "to make motorways as safe as possible".
On a stretch of M1 smart motorway in South Yorkshire, the hard shoulder has been replaced by an active lane and drivers who break down are encouraged to pull in to emergency stopping places.
In a statement, Dr Billings said: "I do not believe there is anyone who uses this stretch of the motorway, as I do, who does not feel anxious when driving along it."
He also highlighted a crash on Friday on the northbound M1 between junction 30 and 31 which he said involved a lorry hitting "a stationary car in a live running lane".
As a result, both carriageways were closed for a time, with motorists experiencing long delays.
The accident is currently subject to a police investigation, Highways England said.
Dr Billings said: "I call upon the minister and Highways England to abandon this type of smart motorway before we have more serious injuries or fatalities."
He added that he had been contacted by lorry drivers concerned over the dangers of stationary vehicles in a motorway lane and the difficulties of being able to pull out into fast-moving traffic.
He said he had written to the transport secretary over his concerns.
Responding to Dr Billings, a Highways England spokesperson said: "We want to do everything we can to make our motorways as safe as possible.
"We are aware of the ongoing concerns from Dr Billings and others and we are working hard to deliver the improvements set out in the transport secretary's action plan."
In March, the government published a report which found that "in most ways smart motorways are as safe as, or safer than, conventional ones", the agency added.
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