The Taliban were among 140 Afghans arrested during an operation ordered by the Baluch government and carried out over the past two days.
Afghanistan, the United States and other Nato powers have been calling on Pakistan to crack down on Taliban fighters operating from the region. Many Taliban fighters settled in the regional capital Quetta after they were removed from power in 2001.
According to police, almost all of them were Taliban fighters, though some were held because they did not have proper documents.
"All of them are Taliban and veteran fighters, not seminary students. They are Afghans and were living here illegally," said Salman Saeed, deputy chief of police in the province.
Most were seized from Islamic religious schools – madrassas - on the outskirts of Quetta.
Saeed said there would be more raids elsewhere in Baluchistan in the next few days.
Police said Mullah Hamdullah, a former commander of the Taliban forces in the southern Afghan province of Helmand, was among those captured in Quetta on Monday.
"We are questioning Hamdullah about the activities he had been carrying out in Pakistan and his linkages with other terrorist groups," police said
Orders for the operation came from the provincial government, a coalition that includes pro-Taliban Islamists. Officials have spoken of growing impatience with Afghans in Quetta, while stressing they were not after genuine refugees.
"The cabinet, last week, instructed the law enforcement agencies to drive them out of the province. They are troublemakers in Pakistan as well as in Afghanistan and all of them will have to go back," said Raziq Bugti, a spokesman for the Baluchistan government.
Arrests of Taliban in Pakistan have been relatively rare, leading to accusations that it has been soft on the Taliban.
President Pervez Musharraf's government backed the Taliban before 2001.
Afghanistan criticised Pakistan's inaction earlier this year, but Pakistan said Afghan intelligence was out of date and the rising violence was being led from inside Afghanistan.
The Taliban movement was formed in Pakistani madrassas in the early 1990s, and talib means student in the Urdu language.