Speaking three days after his government's unilaterally held independence referendum was marred by police violence, Carles Puigdemont said Catalans were united as never before but added he was bitterly disappointed by the king's intervention.
More than 2.2 million people were reported to have voted, according to Catalan authorities, out of 5.3 million registered voters. Many demonstrated in front of the Barcelona headquarters of the Spanish national police. Some 900 people were injured on polling day when police fired rubber bullets and charged at crowds with truncheons to disrupt the vote.
The threat of secession by Catalonia, which accounts for about 20 percent of the country's entire economic output, is also piling political pressure on Spanish Prime Minister Mariano Rajoy and his minority government.
Puigdemont called on Madrid to remove its police forces, which Catalans criticized as having overreacted on Sunday, and said that he would open an investigation into their actions.
Berlin said on Wednesday that it hoped tensions between Madrid and Catalonia would soon calm down, but emphasized the conflict was an internal Spanish matter.
Two girls, one wearing a Catalan independence flag and the other in a Spanish flag, walk in Barcelona, Spain, Tuesday Oct. 3, 2017.
Under the referendum legislation passed by the Catalan parliament, the regional government has 48 hours after the result is finalized to declare independence from Spain.
The Catalan leader said all the votes from overseas would arrive and probably be counted by the end of the week.
Metro stations shut down in Barcelona, pickets blocked dozens of roads and state workers walked out in response to a call for a general strike by pro-independence groups and trade unions.
"This moment calls for mediation".
He said: "Someone needs to tell the Catalan people the truth". "We only received violence and repression as an answer".
"The pictures which reached us from Spain yesterday show how important it is to stop the spiraling escalation now", said German Foreign Minister Sigmar Gabriel.
"I am here because I want Madrid to hear we are not exhausted and we will not accept to repeat the history of fascism", Francesca Carbonell, a 30-year-old waitress in Barcelona, told ABC News.
If Puigdemont does declare independence, a "transition period" will begin.
People shouted "Long live free Catalonia, we are peaceful people and we only want to vote".
In Madrid, officials considered the vote a provocation against Spanish sovereignty and Spain's Ministry of Interior called for an emergency meeting.
European Commission's First Vice President Frans Timmermans said: "It's time to talk".
"Such a declaration would plunge the country into an extraordinarily complex situation with unknown, but very serious consequences", the group said in a statement. It said it trusted Rajoy "to manage hard process" in respect of the Spanish constitution.
Catalan separatists face several major hurdles to having the vote recognized as legitimate, in Spain and overseas, though for them, simply holding the referendum amounted to a victory of sorts.
In a rare televised statement, King Felipe said the referendum's organizers had jeopardized national stability.