The 88-year-old's death on Monday after a serious health battle was marked by tolling church bells and preparations for scores of memorial masses for the leader ahead of his funeral on Saturday.
Outside St Patrick's Cathedral in Melbourne, Archbishop Peter Comensoli described Pope Francis as someone who took a personable approach to the role.
Archbishop Comensoli met with the pontiff several times, most notably when he was appointed into his role in Melbourne in 2018.
"He knew me personally ... whenever you engaged with Francis it was direct, it was an encounter, one to one," he said.
"Even when there were a whole lot of other people, he honed in, for a short moment, but he did that."
Archbishop Comensoli said Pope Francis had the ability to listen and respond to others.
He jokingly spoke of a time where he penned a letter to the Pope, while passing through Rome.
Archbishop Comensoli was leading a group of young people who were attending the World Youth Day in Lisbon in 2023 and had asked for a meeting on a whim.
"He said yes, amazingly," he said.
"These young people had an hour with him. He said 'ask me questions'. He was so open to it and so engaged. It was very beautiful."
Archbishop of Sydney Anthony Fisher, who met Francis about 20 times, described the Pope as very easy to talk to and almost like "an Australian in terms of his informality".
"He shared a real passion for the marginalised, for refugees, for people who felt alienated from society, for people who were poor, financially and emotionally," he told ABC TV.
Many mourners attended early masses at local cathedrals following the Pope's passing.
Adam Wojcik, 30, said Pope Francis' time at the helm made him hopeful about the future of the church while paying his respects at St Patrick's Cathedral on Tuesday.
"I am a gay man as well and this is weird for me to kind of connect with the church like this," he told AAP.
"Something has really moved me about Pope Francis.
"I just hope that whoever comes next, carries that same message of hope for humanity, especially in this tumultuous, crazy world."
Outside Sydney's St Mary's Cathedral, Stephen said Francis had continued Pope John Paul II's legacy as a man of the people.
"That's what Pope Francis brought to this world: really giving everyone hope and not just making the church something that's symbolic," he told AAP.
Prime Minister Anthony Albanese said the major party leaders had agreed to dial back election campaigning on Tuesday as a sign of respect.
He attended mass at St Patrick's Cathedral in Melbourne on Tuesday morning.
Anglican Archbishop Geoffrey Smith said Pope Francis was a man of "great humility and humanity".
"Not only did he dedicate his life to serving the poor and standing up for those facing persecution, he was a great advocate for peace during these unsettling times," he said.
National flags on government buildings flew at half-mast on Tuesday as a mark of respect.
Cardinal Mykola Bychok said he was filled with sadness for the loss of a "Pope of peace" and a man of simple piety.
He was on his way to the Middle East on a pilgrimage but will divert to Rome to take part in the funeral rites before joining other cardinal electors to choose the 267th and next pope.
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