Khaled abu Arafeh and Mohamed Totah were arrested at a Red Cross compound where they had been conducting a sit-in for the past year and a half.
Israeli police spokesman Micky Rosenfeld told CNN the two men, whom he described as Hamas activists and residents of East Jerusalem, "are being investigated and will later be taken to court."
"They are not immune from the law," Rosenfeld said.
Last week, Israel arrested two other Palestinian Legislative Council members in the West Bank -- Aziz Dweik and Khaled Tafesh Dweib -- for what the Israeli military said was involvement in terrorist activity.
The latest round of arrests brings the number of Palestinian parliament members imprisoned by Israel to 27, according to Addameer, a Palestinian prisoner advocacy organization. Israeli authorities could not immediately provide a count.
Sabri Saidam, a senior adviser to Palestinian Authority President Mahmoud Abbas, told CNN, "It is impossible for the free world to see a state claiming to be wanting peace by attending talks in Amman, while kidnapping legitimate parliament representatives and elective members of the Palestinian society ... . This act is a demonstration of the real wish of the Israeli government to cripple any efforts in the direction of achieving a lasting peace in the region."
Cecilia Goin, a spokeswoman for the International Committee of the Red Cross, confirmed that Arafeh and Totah had been arrested at the compound at around 1:15 p.m. (6:15 a.m. ET).
In July 2010 Arafeh, Totah and another Palestinian legislator named Ahmad Atun entered the compound and began an open-ended sit-in according to Goin.
Israeli police arrested Atun in September, but the other two parliament members remained.
The ICRC said at the time the men sought refuge in the compound that it notified Israeli authorities of their presence. The ICRC said it informed the two that the organization held no diplomatic status in Israel and could not protect them from arrest.
On Friday, after the arrest of Dweik and Dweib, Hamas leader Ismail Haniyeh called on Abbas to halt talks with Israel.
"There should be a stop to the ongoing negotiations. The negotiations are a failure and absurd. It is impossible for any Palestinian to shake the hands of the occupier and the enemy while they are arresting the symbols of legitimacy," Haniyeh said.
Due to political divisions between Palestinian political factions, the Palestinian Legislative Council has not met since 2007.