"Given the scale of the crisis and the suffering of the people, today I can announce that we will do more - providing resettlement for thousands more Syrian refugees," Cameron said in Lisbon after talks with his Portuguese counterpart, Pedro Passos Coelho.
"We will continue with our approach of taking them from refugee camps. This provides them with a more direct and safe route to the UK rather than risking the hazardous journey which has tragically cost so many of their lives," he said.
No specific figure has been given but the UN refugee agency said the UK would take a further 4,000 Syrian refugees.
"Britain will act with our head and our heart, providing refuge for those in need while working on long-term solutions to this crisis," Cameron told reporters.
His announcement followed a firm buildup at home and abroad to show more humanity, especially after the publication of disturbing images of a three-year-old Syrian boy found dead on a Turkish beach.
The migrant crisis, with the number of people fleeing the volatile Middle East for Europe increasing every day, has been described as the largest exodus of people since World War II.
Mounting calls from the international community for Britain to do more ensued as Cameron earlier said taking in any more refugees was not the answer.
"As I said earlier in the week, that means bringing an end to the conflicts that are driving so many to flee, including the bloodbath that has engulfed Syria," Cameron said.
He, however, defended UK's response to the crisis so far, saying its 900-million pounds aid given to Syria, including food and medical supplies, stopped greater numbers from trying to reach Europe.
UK development charity Oxfam welcomed indications of a shift in the government's policy.
"Offering to resettle 10,000 Syrian refugees would bring the UK in line with other European countries who have already shown leadership in offering a haven to vulnerable refugees," said chief executive Mark Goldring.
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