The United Nations said security forces have killed more than 50 people to stamp out daily demonstrations and strikes in the South-East Asian nation since the military overthrew and detained elected leader Aung San Suu Kyi on February 1.
In a statement released on Sunday night, Foreign Affairs Minister Marise Payne flagged the government's "grave concerns" about the "escalating violence and rising death toll" in protests against the coup.
"We condemn the use of lethal force or violence against civilians exercising their universal rights, including the right to freedom of expression and peaceful assembly," she said.
"We continue to strongly urge the Myanmar security forces to exercise restraint and refrain from violence against civilians."
On Sunday, there were reports that live bullets, as well as tear gas, were used by security forces to disperse thousands of protesters in cities across Myanmar.
As a result of this sort of violence, Australia will pause a military program with the country.
"Australia has had a limited bilateral Defence Cooperation Program with Myanmar's military, restricted to non-combat areas such as English language training. This program will be suspended," Payne's statement read.
It comes days after documents released under freedom of information laws revealed new details about Australia's controversial program of defence cooperation with Myanmar's military.
Australia is one of a small number of nations that maintained cooperation with Myanmar's armed forces - known as the Tatmadaw - in the wake of a brutal 2017 campaign of ethnic cleansing waged against the Rohingya minority.
Human rights groups have long campaigned against the program, and calls for it to be axed have intensified since the military seized power last month in a coup.
Pressure on the government has continued to mount over the past two weeks as the Tatmadaw cracked down on pro-democracy protesters.
The Australian government will redirect humanitarian aid towards vulnerable groups, including the Rohingyas and other ethnic minorities, with an Australian development program no longer going through any of Myanmar's government bodies.
"We will prioritise the most pressing humanitarian and emerging needs and seek to ensure our humanitarian engagement is with and through non-government organisations, not with government or government-related entities, as is currently the case in some parts of the program," the statement read.
Australian professor Sean Turnell has also "been detained with limited consular access" for more than a month.
Payne reiterated the government's call for the release of Professor Turnell, as well as former Myanmar leader Aung San Suu Kyi, President Win Myint "and others who have been arbitrarily detained since 1 February".
"We call on the Myanmar regime to engage in dialogue," the statement read.
"Australia will continue to play a constructive role, including in consultation with international partners, particularly ASEAN, in support of the Myanmar people."
Sunday's protests, held in at least half a dozen cities, marked some of the most widespread action against last month's coup and security forces used tear gas, stun grenades and, according to several residents on social media, live bullets to break up the demonstrations.
"They are killing people just like killing birds and chickens," one protest leader said to a crowd in the southern town of Dawei.
"What will we do if we don't revolt against them? We must revolt."
A local campaign manager for Suu Kyi's National League for Democracy died in custody after being arrested in the country's largest city of Yangon over the weekend, according to a legislator from the now dissolved parliament.
Well over 1700 people have been detained under the junta by Saturday, according to figures from the Assistance Association for Political Prisoners (AAPP) advocacy group.
"Detainees were punched and kicked with military boots, beaten with police batons and then dragged into police vehicles," AAPP said in a statement.
"Security forces entered residential areas and tried to arrest further protesters, and shot at the homes, destroying many."
The state-run Global New Light Of Myanmar newspaper quoted a police statement as saying said security forces were dealing with the protests in accordance with law and tear gas and stun grenades were used to break up riots that were blocking public roads.
Protesters demand the release of Ms Suu Kyi and the respect of November's election, which her party won in landslide but which the army rejected.
The army has said it will hold democratic elections at an unspecified date.
Students and community members have launched the Anti-Myanmar Military Dictatorship network.
Mary Aung, a student activist and part of the Anti-Myanmar Military Dictatorship Network, said she welcomed Australia's latest move.
On Saturday, the group had launched a petition calling on the Australian government to "suspend all high-level contact with Myanmar's military officials".
"Australia is on the right track even though there are more actions that still need to be taken, such as recognising CRPH as the government, and imposing more targeted financial and economical sanctions," she told the ABC.
"But it's at least a good step."
Myanmar students have also called on businesses to cut ties with the military and their associates, due to human rights being "brutally crushed" in the country.
"I am part of Gen Z, and this was the first time we started voting, and this is how we were respected? Our voices were disrespected," Kyi Phyu Moe Htet said at the Melbourne launch.
"I can't go back home … the only response from the military will be to put us into jail or to suppress our voices. So we're not going to stay silent. We will not do that. We will never, never stay silent."
Christopher Lamb, the former Australian ambassador to Myanmar during the late 1980s - when an earlier student uprising against military dictatorship was violently suppressed - said he didn't see the current takeover as a "coup".
"A coup is usually something which is final, and which we have no choice but to accept. I don't see this as final," he said at the Melbourne event.
"There is such a strength in the people... and I don't see how this takeover can endure. The time will come when this is brought undone."