Protesters across the country have demanded an end to armed police in remote Indigenous communities.
Saturday's marches follow the March after he fatally shot Aboriginal teenager Kumanjayi Walker, who was armed with scissors.
Ahead of the protests, Warlpiri elder Ned Jampijinpa Hargraves, from the remote Top End town of Yuendumu where Mr Walker died, said police with guns only caused fear.
"We cannot accept that anymore. We don't want to feel terrified in our own ngurra, our own home," he said.
Protesters at Sydney's Town Hall on Saturday, 18 June, 2022. Source: SBS News
"Over 500 First Nations people have died in custody since then," the union said.
Protesting in Sydney were Darlene Mason and Mark Mason Jnr whose father Mark Mason was shot by police in a remote Indigenous community in 2010. Credit: SBS News
"I'm here to stand up against the violence that's been done to us in the communities all the way across Australia," Teresa Monta told SBS News.
"Because we're being badly handled on the streets by the way of the institutional racism which is happening within the police forces. Then when it gets into the courts, you know, we have this mentality of we're always at fault.
"Whether it be our children or our women or our men, all the worst is thought of us, you know, and the worst punishments are dished out to us."
Auntie Rhonda Dixon-Grovenor rallying against gun use in Indigenous communities, Sydney 18 June, 2022.
"Not long ago, a 19-year-old young man was killed and it really hurts me because I've got 14 grandchildren, and I have a 19-year-old grandson," Ms Dixon-Grovenor said.
"When one of our people suffer, we all suffer.
"We're only two per cent of the population. And yet 40 per cent and higher are incarcerated, and this violence and this racism is going to stop.
"There's no need to have guns in the communities," she said.
"There needs to be better training for the police and they should understand our history and how to communicate with Aboriginal people."
The "ceasefire" being called for by protesters would include defunding Northern Territory police, redirecting their funding to community-based services and demands for Mr Rolfe to face "customary law" in Yuendumu.
Elders also demanded an end to any lingering powers from the 2007 Northern Territory intervention.
"This is not only for Warlpiri people, this is for everyone. For all our First Nations peoples, our warrmala, it is time for us to stand together," Mr Hargraves said.
Marches were held from Sydney to Perth, with protesters on Friday blockading a Brisbane facility of a weapons manufacturer that supplies the Northern Territory police.
In Alice Springs, protesters marked 15 years since the NT Intervention.