Most Revd Justin Welby had "tears running down" his face whilst listening to the radio and reading the newspaper as the plight of thousands of refugees trying to reach Europe is revealed.
He said he has a "sense of deep frustration" and wondered "what can we do more?".
"Our track record in the Middle East, in terms of effort on the ground in the refugee camps has been extraordinary, second only to the United States," he said.
"In the end though, it comes down to finding ways of getting people who would otherwise be dying into places of safety and security with a hope of a future."
Archbishop Justin said he was "very pleased" and welcomed the news that Britain will take "thousands more" refugees from camps on the borders of war-torn Syria.
Prime Minister David Cameron said he would set out details of the plans next week and that Britain had a "moral responsibility" to help refugees.
Archbishop Justin said: "It's not just about money or numbers, it's about the reality of human beings.
"It is essential there is a European response, every nation in Europe has to bear the burden proportionally as much as they are able.
"We can't do what we can't do, but we must do what we can."
Mr Cameron said: "We have already accepted around 5,000 Syrians, and we've introduced a specific resettlement scheme alongside those we already have to help those Syrian refugees particularly at risk.
"As I said earlier this week, we will accept thousands more under these existing schemes, and we keep them under review. Given the scale of the crisis and the suffering of people, today I can announce that we will do more, providing resettlement for thousands more Syrian refugees.
"We will continue with our approach of taking them from the refugee camps. This provides them with a more direct and safe route to the United Kingdom, rather than risking the hazardous journey which has tragically cost so many their lives."
A spokeswoman for the United Nations refugee agency suggested the UK will take 4,000 more refugees from Syria - though there was no confirmation of this from Downing Street.
"We obviously welcome very much the move to increase resettlement spaces for Syrians in the UK. Those spaces are going to be critical to the lives and future of 4,000 people," said UNHCR spokeswoman Melissa Fleming, adding that there was "momentum" for other countries to follow Britain's example.
Ukip leader Nigel Farage said the majority of those crossing the Mediterranean were economic migrants, and that nothing should be done to encourage them to make the journey.
Speaking at the launch in London of his party's Say No campaign for the referendum on Britain's EU membership, Mr Farage said: "The EU has got this wrong. Anybody that comes, from whatever background and virtually for whatever reason, can claim to be a refugee.
"If the European Union wants to help genuine refugees, they need to establish offshore centres and process people correctly, rather than inviting what has now turned into a headlong rush."