Federica Mogherini said there had to be more co-operation both with Muslim countries and internally within the EU.
The Brussels summit follows gun attacks in Paris that killed 17 people and anti-terrorism raids in Belgium.
Two of the Paris gunmen said they were “avenging” French cartoons of the Prophet Muhammad.
Tens of thousands of people rallied on Monday in Grozny, capital of Russia’s mainly Muslim region of Chechnya, to protest against the cartoons published in Charlie Hebdo magazine.
The foreign ministers were meeting ahead of a special leaders’ summit on terrorism on 12 February.
Ahead of the Brussels talks, Ms Mogherini said: “The threat is not only the one we faced in Paris, but is also spreading in many other parts of the world, starting from Muslim countries.
“We need to strengthen our way of co-operating together first of all with Arab countries and then internally. We need to share information more, we need to co-operate more.”
Arab League Secretary General Nabil al-Arabi is attending the talks with the 28 EU foreign ministers.
Ms Mogherini said: “We will discuss with the secretary general how to increase the level of co-operation… we need an alliance, a dialogue.”
UK Foreign Secretary Philip Hammond echoed her call, saying Muslim countries had “suffered the greatest burden of terrorism”.
High on the agenda of the talks will be concerns surrounding the return of radicalised Europeans who have gone to fight in Iraq and Syria.
Mr Hammond said specific measures to be discussed would include “passenger name records within Europe”.
Other measures believed to be on the table are tighter border controls within the Schengen area and the fight against illegal arms-trafficking.
EU interior ministers will discuss their response when they gather in Riga on 29 January.
On Thursday, members of the US-led coalition against Islamic State will meet in London. US Secretary of State John Kerry will attend.
The Brussels talks come after anti-terror raids in Belgium, France and Germany led to more than 20 arrests.
Belgian police killed two suspected jihadists in the town of Verviers last Thursday and five people arrested were with “participating in the activities of a terrorist group”.
Several people were also arrested in the Greek capital, Athens, on Saturday. Belgium is asking Greece to extradite one of the suspects over a possible link with the alleged Belgian plot.
Belgian police are still searching for Abdelhamid Abaaoud, the alleged leader of the cell suspected of planning to kill Belgian police officers.
No link has been established between the Belgian case and last week’s attacks in France.
Gunmen in Paris killed 12 people at the offices of satirical magazine Charlie Hebdo, a policewoman and four hostages at a kosher supermarket. The three gunmen involved were shot dead by police.
The attacks drew international outrage and a huge anti-terrorism rally in Paris attended by many world leaders.
The first issue of Charlie Hebdo published after the attacks carried a new cartoon of the Prophet on its cover, sparking angry protests in parts of the Muslim world, including Pakistan and Niger.
Monday’s rally in Chechnya drew people from various Russian regions, BBC Russian correspondent Yuri Vendik in Grozny reports.
At least 350,000 people appear to have turned out although Russian police put the figure at 800,000.
Many demonstrators carried signs such as “Hands off our beloved Prophet Muhammad”. The rally was also anti-Western in character, our correspondent says.
In Gaza City, Hamas allowed a demonstration against the magazine by Salafists, at which a French flag was burnt.
In another development, the EU said it would appeal against a European court ruling last month that it must remove the Palestinian group Hamas from its list of terrorist organisations.
As a result of the appeal, Hamas will remain on the list and its assets will stay frozen pending a judgment by the Court of Justice, the highest legal authority.