Nicola Sturgeon said a “dialogue” between the two sides was now needed as she condemned the violence which took place during Sunday’s vote.
She stopped short of suggesting an agreement on another ballot, but said “in any democracy there has to be surely a legal way for people to express their view”.
Hundreds of people were injured when national police tried to stop voting in the poll which was deemed illegal by the Madrid government and the country’s top court, but was backed by the Catalan regional authorities.
Catalan officials said 90 per cent of the 2.26 million people who took part in the vote backed independence. The region has 5.3 million registered voters.
Speaking during a visit to Aberdeen, Ms Sturgeon said: “I think dialogue now has to replace the kind of confrontation we have seen.
“Not withstanding the many hurdles the referendum process faced and the scenes we saw yesterday, the overwhelming majority of people who did vote yesterday voted for independence.
“Spain is of the view and will maintain the view that that vote was not in line with its constitution and therefore isn’t legitimate.
“While that’s the position of Spain, I understand that, you cannot simply ignore the kind of strength of feeling that we’ve seen expressed.
“I hope now that there is a process, a dialogue, that will allow both the Spanish and Catalonian governments to find a way forward that respects the rule of law, respects democracy but also respects the right of the people of Catalonia to decide the future of their country.”
Asked if she thought there should be an agreement on holding a legal referendum, Ms Sturgeon added: “Look that’s not for me to say.
“I think in any democracy there has to be surely a legal way for people to express their view and therefore there should be a process of dialogue that allows Catalonia and the Spanish Government to decide the way forward here.
“We saw yesterday a very significant expression of support for independence for Catalonia and that can’t simply be cast aside.”
The First Minister also repeated her criticism of the response from the UK Government, which she described as “shamefully weak” over the weekend.
The Foreign Office said the referendum was “a matter for the Spanish government and people”.
“I think all democrats watching those scenes yesterday would have been horrified, and I thought the statement from the Foreign Office should have been stronger in saying that kind of behaviour was not acceptable,” Ms Sturgeon said.
“A real friend to Spain and I count Scotland as a friend to Spain I think should say that that kind of behaviour doesn’t do the reputation of Spain any good.”