Almost 5,000 trolleys were dumped across the city's housing estates last year.
Up to now they have been collected by city council contractors and returned to supermarkets.
But from this month trolleys will be seized by the council and supermarkets will have to pay £9.47 per trolley to get them back.
If they don't pay within six weeks, the trolleys will be disposed of.
Cllr Jason Fazackarley, who is charge of environment and community safety issues at the council, said: 'We have spoken to supermarkets and understand that they take the situation seriously and have improved the security of trolleys.
'But the fact is that thousands of them are still being dumped on our housing land – about 3,000 so far this year.
'We are also asking residents who dump trolleys to stop.
'Abandoned trolleys spoil the environment for their neighbours, cause obstructions – especially for disabled and elderly people – and can cause damage.'
Havant Borough Council started fining supermarkets £50 for dumped trolleys last year – and it has had an impact.
Before, up to 40 a month were found littering the streets but in May there were just five, while in June there were none.
Councillor David Collins, who is in charge of environment matters at Havant council, said: 'It's the same as anything – once there is money involved it doesn't take a long time to improve.
'It has had a terrific impact – the number of abandoned trolleys has significantly reduced.'
Portsmouth City Council plans to get even tougher from January next year when supermarkets could face even higher fines.
Clive Rankin, Portsmouth's clean city manager, said: 'Essentially at the moment we are just aiming to cover our costs for recovering the trolleys.
'But in the future we will be able to recover all associated costs, such as storing the trolleys or disposing of them.
'Some supermarkets are already trying to do something to improve it, but we still have significant numbers of trolleys dumped and they do cause a problem.'