Rebels stormed the regional police building and town hall in the eastern Ukrainian city of Gorlivka, local officials said, adding to more than a dozen locations already under their control.
The new seizure followed clashes in nearby Lugansk yesterday, as hundreds of pro-Russia protesters spearheaded by a heavily armed mob attacked the police station.
Today, the rebels lifted their siege of the HQ building after the police chief promised to step down.
Ukraine's interim president Oleksandr Turchynov told his cabinet that the nation's law enforcement bodies were "helpless" to prevent the insurgents storming official buildings in the restive east.
Also Read
Turchynov urged Ukrainian "patriots" to bolster the beleaguered police force, which he has criticised for "inaction and in some cases treachery".
He warned also that there could be "acts of sabotage" by Russia during public holidays at the beginning of May.
The defence ministry announced that the security services would hold drills in central Kiev overnight but this was not expected to involve military hardware.
Yulia Tymoshenko, a former prime minister who is a frontrunner for presidential elections on May 25, said Russia had already started an "undeclared war" against her country.
The West has accused Russia of fomenting the crisis and backing the rebels and has imposed sanctions to try to get Moscow to back down.
President Vladimir Putin insisted late yesterday that there were "neither Russian instructors, nor special units, nor troops" operating in Ukraine.
The separatists have vowed to hold a referendum on closer ties with Russia on May 11.