The pair made a surprise trip to Baghdad from the UK on Sunday, after Ms Rice's two-day stay there hosted by Mr Straw.
The talks with Iraqi PM Ibrahim Jaafari and President Jalal Talabani come as Iraqi politicians are struggling to form a government of national unity.
Speaking to reporters travelling with her to Iraq, Ms Rice said: "The fact that we're going out to have these discussions with the Iraqi leadership is a sign of the urgency which we attach to a need for a government of national unity." She added it was "important to have fresh messages from time to time from Washington and from London".
Ms Rice and Mr Straw also met Vice-President Adil Abdul Mahdi and other Iraqi leaders.
The visit came amid continuing violence in Iraq:
At least four bodies were found in the Iraqi capital, Baghdad
Insurgents were reported to have blown up a small Shia mosque in the village of Kibba near Baquba, north-east of Baghdad, but there are no reports of any casualties
Six insurgents were killed in an explosion in a house on the southern outskirts of Baghdad. Police said they died when a bomb they were preparing exploded prematurely
Four other insurgents were killed in two failed attacks against American and Iraqi forces near Balad, north of Baghdad, the US military said
Two pilots of a US helicopter that crashed after coming under hostile fire on Saturday are presumed dead, the US military said
Two US soldiers were also killed by a roadside bomb while on patrol in central Baghdad late on Saturday
BBC
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