Spain's Constitutional Court on Thursday ordered a suspension of Catalonia's parliamentary session next week during which the region has said it might declare independence and further fuel Spain's worst crisis in decades.
Mr Vargas Llosa is also among 60 Spain-based intellectuals and academics who have signed an open letter asking the worldwide community not to support the idea of external mediation as a solution to the crisis in Catalonia.
Demonstrators dressed in white gathered outside city halls in Barcelona, Madrid and across Spain on Saturday to demand the two sides stop sparring and hold talks.
Hundreds of people are gathering in downtown Barcelona ahead of a rally to protest the Catalan government's push for secession from the rest of Spain.
"It is evident that we will take whatever decision that we are permitted to by law, in view of how things are unfolding", Rajoy told the El Pais newspaper in an interview.
The Spanish official added that the Catalan movement aimed at obtaining more autonomy for the region should be peaceful and be conducted "within the framework of treaties".
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After days of ill-tempered rhetoric, Madrid said it regretted the injuries caused in the October 1 crackdown and suggested Catalonia should hold a regional election to settle the crisis.
After a referendum over independence was held last Sunday, several companies chose to move their headquarters away from this Spanish northeastern region, Xinhua news agency reported.
"It's reached a turning point and we need to get actively involved in the defence of Spain's values as a nation", added 52-year-old Joaquin Penas, an off-duty cavalry colonel with a Spanish flag draped round his shoulders.
Recent polls had indicated that Catalans are split on independence, though leaders said the violence during the referendum turned many against the state authorities. Hundreds of people were hurt as police, trying to enforce a Spanish court ban on the vote, attempted to seize ballot boxes and disperse voters. He says he has an opinion about Catalonian independence, but that is not what is called for here.
Valls questions the wish of Catalan leader Carles Puigdemont to pull the region from the country, saying they would be leaving the European Union if they did so.
It is unclear whether he will declare independence.
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Raul del Hoyo, 56, a logistics technician, said he feels Spanish as well as Catalan but believes in the region's bid for independence.
"If there is a unilateral declaration of independence, that will be that".
In a separate rally in Madrid's Colon Square, thousands clamored for the unity of Spain and against any attempt by the northeastern region to break away.
"Besides Catalans, there are thousands of men and women from all corners of Spain who have come to tell their Catalan companions that they are not alone", said Llosa, who took on Spanish citizenship in addition to that of his native Peru in 1993.
There is no doubt the majority of the people do not want independence.
While Rajoy has said he needs "to do everything in the right time".
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The dispute escalated Wednesday, culminating with the attack about 30 minutes into a history class. She plans to pull her daughters out of school.
He did not rule out suspending Catalonia's regional autonomy - a move that could risk sparking unrest.