The European Union’s Brexit coordinator launched into a scathing attack following Sunday’s referendum, which saw hundreds of people injured in violent clashes.
And he called any declaration of independence “totally irresponsible” and warned “it’s not a shame to make compromises.”
In a speech in the European Parliament today Mr Verhofstadt said: “To my friends in Catalonia I want to say it is not in your interest to pursue separatism at all costs.
“The point is this referendum lacked basic democratic legitimacy.
“You know very well in advance the majority of people would not participate, stay at home, as the majority do not believe in independence, and it is not by accident you did not install a minimum threshold.
“The result was already known before it begun. What do you call this? Manipulation, deception.
“Moreover though to declare independence based on a defective referendum is irresponsible.”
Mr Verhofstadt, a Liberal former prime minister of Belgium, also blasted referendum organisers for failing to go beyond legal arguments to find genuine dialogue and compromise.
He said: “I think now Spanish democracy has to surmount itself again, to surmount this deep division, to overcome this crisis.
“And I think it has to do so not by believing the judiciary can solve the problems on its own and certainly not by violence.
“And not just by relying on the power of the state.
“No, what we need is a new political vision, inclusive dialogue.
“A vision that the future and our people living in Spain lies in a multicultural, multilingual federal state embedded in a multicultural, multilingual federal Europe.
“It is true you cannot go against the law and it is also true you cannot govern with the law.
“But you cannot solve such deep divisions only with the law.
“To try to understand each other, to dialogue, to talk with another and that is the only way to find solution and that is the real strength of good politicians and statesmen.”
His comments come as the EU executive called again for the Spanish government and Catalan authorities to open dialogue to defuse the violence and civil unrest in Catalonia.
The European Commission’s deputy head, Frans Timmermans, told the European Parliament during an emergency debate on the crisis in Spain: “It’s time to talk.”
Sunday’s vote has plunged Spain into a major constitutional crisis .
Spanish Prime Minister Mariano Rajoy is struggling to secure support from across the traditional political divide in his battle to stop Catalonia breaking away – a lack of consensus that could compound Spain’s worst political crisis for decades.
Rajoy is mulling the unprecedented step of invoking the constitution to dissolve the Catalan parliament and trigger regional elections, ruling party lawmakers say.
Participants in the referendum opted overwhelmingly for independence, but turnout was only about 43 percent given that Catalans who favour remaining part of Spain mainly boycotted the ballot.