Tony Blair says he told Vladimir Putin "people were becoming fearful" of Russia's foreign policy.
Mr Blair said the atmosphere was cordial with Mr Putin
During "very frank" talks at the G8 summit, Mr Blair said President Putin expressed concern Russia "was not being treated properly by the West".
And Mr Blair expressed "our view that people were becoming worried, fearful about what was happening in Russia today, the external policy".
Tensions have been high after Mr Putin talked of aiming missiles at Europe.
Mr Putin is concerned about plans by the US to site missile defence systems in Poland and the Czech Republic.
Mr Blair said the pair spoke for about an hour on the fringes of the G8 summit in Germany.
He told reporters: "It was a very frank discussion.
"It went through all the issues you would expect us to go through and we set out each other's views, which are well known.
"The atmosphere on a personal level was perfectly cordial but there are real issues there and I don't think they will be resolved any time soon."
They spoke about energy, missile defence systems and the murder of Russian ex-spy Alexander Litvinenko.
In an earlier meeting with US President George Bush, Mr Putin suggested that the US could use a former Soviet radar base in Azerbaijan, instead of placing missiles in Poland and a radar base in the Czech Republic.
Such a compromise could prompt Russia to withdraw its threat to re-target Russian missiles at Europe, Mr Putin said.
In his meeting with Mr Blair, the Russian President talked about his country's refusal to extradite former KGB agent Andrei Lugovoi over the murder of Alexander Litvinenko in London.
Elsewhere at the summit, Mr Blair said "immense progress" has been made on aid to Africa by the G8.
Mr Blair said both Africa and the G8 knew they had "a long way to go and a lot to do" but the leaders of the world's richest nations had "recommitted" to an aid deal it made two years ago.
The deal aims to deliver £30bn to fight Aids and provide free schooling in Africa.
"The important thing about what we have agreed today is that we have recommitted ourselves to all the commitments we made a couple of years ago at Gleneagles," said Mr Blair.
"The important thing is we have set out how we are going to do them."
He added: "It's a deal between Africa and the developed world and just as we have recommitted ourselves to substantial increases in support and help, so Africa has recommitted itself to its responsibilities as part of a partnership - proper governance against corruption, proper democracy and so on."