Speaking to hundreds of Syrian refugees along the Jordan River, the pope called for an end to the civil war which has cost more than 160,000 lives, urging "all parties to abandon the attempt to resolve issues by the use of arms and return to negotiations".
Jordan is the first stop on Francis's "pilgrimage of prayer" which continues Sunday in the Palestinian territories and Israel.
His landmark maiden visit to the Holy Land is chiefly aimed at boosting ties with Muslims and Jews, as well as seeking closer unity with Orthodox Christian leaders.
After being greeted by King Abdullah II, Francis received a raucous public welcome from 40,000 pilgrims as he arrived to celebrate a mass at Amman's main international stadium, the biggest gathering of his trip.
Entering the stadium in an open-topped white jeep, he smiled and waved enthusiastically at the crowds, his white skullcap flying off in the breeze.
"Peace is not something which can be bought, it is a gift to be sought patiently and to be crafted through the actions, great and small, of our everyday lives," he told the crowd packed into a sea of blue and red chairs on a sweltering May afternoon.
The 77-year-old pontiff called on the world to help Jordan deal with its "humanitarian emergency" caused by a massive influx of 600,000 refugees from neighbouring Syria.
Abdullah himself drove the pontiff a couple of kilometres in a golf cart to the reputed site of Jesus's baptism on the River Jordan, chatting avidly to Francis who was squeezed in besides him, in another sign of the pontiff's famed informality.
At two different sites along the riverbank, Francis stood for a few minutes in silent prayer, his head bowed, before being driven on to meet and pray with 600 Syrian and Iraqi refugees, who told him of their suffering.
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