"On day one, I am going to begin swiftly removing criminal illegal immigrants from this country - including removing the hundreds of thousands of criminal illegal immigrants that have been released into US communities under the Obama-Clinton administration," Trump told supporters in Des Moines, Iowa, on Saturday.
The business mogul, who earlier this week softened on his immigration plan, said he would also deport those who overstay their visas.
He said he would launch a tracking system to find those whose visas have been expired so that they are removed quickly.
Trump also doubled down on the most controversial aspect of his immigration policy – building a towering wall along the US-Mexico border.
"I am going to build a great border wall, institute nationwide e-verify, stop illegal immigrants from accessing welfare and entitlements and develop an exit-entry tracking system to ensure those who overstay their visas are quickly removed," Trump said.
Trump, however, did not elaborate on how he would install a "deportation force" to deport 11 million undocumented immigrants, some of whom have been in the country for decades.
He also linked illegal immigration to unemployment affecting US citizens, including African Americans.
"Every time an African-American citizen, or any citizen, loses their job to an illegal immigrant, the rights of that American citizen have been violated," he said.
He criticized his Democratic rival Hillary Clinton saying, "A vote for Trump is a vote to have a nation of laws, a vote for Clinton is a vote for open borders."
The race for the White House has become tight between the two candidates as a new poll puts Clinton 5 percentage points ahead of Trump in terms of national support, 41 percent to 36 percent.
Nearly 23 percent of likely voters said they would pick neither candidate, according to the latest Reuters/Ipsos daily tracking poll released on Friday.
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