Two 20-year-old men arrested for questioning about the attack on the City Church were released by police on Tuesday night, pending a report to the Public Prosecution Service.
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A third man, also aged 20, was released unconditionally.
A police spokeswoman said following extensive inquiries they were not linking the attack on the church to the attacks on Romanian families and that there was no indication of a hate or racial motive.
Two teenagers, aged 16 and 17, who were being questioned about intimidation and provocative conduct, have also been released on Tuesday night pending further inquiries.
The windows of City Church in the university area were smashed on Monday night.
The three men were arrested hours later at a house a short distance from the City Church in south Belfast's University Avenue for questioning about the attack which was captured on CCTV.
Meanwhile, a 21-year-old man appeared in court in Belfast charged with intimidating Romanians last week.
On Monday, two boys aged 15 and 16 also appeared in court on charges linked to the attacks.
Church vandalised
The City Church provided sanctuary for more than 100 Romanians forced to flee their south Belfast homes.
The damage was discovered by Pastor Malcolm Morgan on Tuesday morning.
He said: "I arrived at 7am and found several windows smashed at the front of our church and the main door windows smashed.
"There were stones lying scattered on the floor inside and outside and obviously broken glass all around."
Mr Morgan said the church had never been attacked in such a way before, but added that it was only speculation that it was connected to the help the church had given to the Romanian families.
"It would be easy to conclude that it was someone who did not like our work with the Romanians, but that is only guesswork.
"If it is, I think that is very sad. We had nothing but positive comments all last week - so many emails and local folk thanking us - so it was quite a surprise this morning," he said.
He said he did not regret what he had done for the migrant workers.
"Absolutely not. I was just thrilled we as a church were able to respond last week and we would do the same tomorrow."
'Shameful'
Deputy First Minister Martin McGuiness branded the attack on the church "totally and absolutely wrong, totally shameful and totally unforgivable".
He said the church and its pastor, Mr Morgan, had been an inspiration in recent weeks and a symbol of goodness in their help for the Romanian families.
It is understood the breaking of the leaded windows was caught on CCTV cameras.
Mr McGuiness added: "One of the things that does concern me over the events in Belfast over the course of the last number of weeks is the slogan shouting of Combat 18 and the writing on walls of Combat 18.
"There are an awful lot of sectarian bigots and racist bigots within our society, of that there can be no doubt.
"What we need to see is a coming together of all the political institutions and the politicians to lead by example."
Mr McGuiness - who visited the church and Mr Morgan with Belfast's Lord Mayor, Naomi Long, to inspect the damage - said that, if politicians did not lead by example and speak with one voice, "We are doomed to revisit this in the coming weeks and months".
South Belfast MLA Anna Lo has also condemned the attack.
She said: "This use of violence, it's really a culture that we need to stop in Northern Ireland.
"People just seem to use violence whenever they don't agree with anything or when they see anyone different and think they can use bullying tactics to get them out."
PSNI Chief Constable Sir Hugh said: "It shows that Northern Ireland still has to come to terms with the fact there are small numbers of people in the communities determined to drag us backwards - it's the new sectarianism, for want of a better description."
He also highlighted the work being done by community advocates to act as points of contact for minority groups and the police.
Security Minister Paul Goggins said more had to be done for migrants to feel confident coming to the region to work.
"I think the attack on a place of worship last night was absolutely to be condemned and I think that the Romanian people know that the people of Northern Ireland by and large are deeply concerned and perplexed by the attacks that have taken place," he said.
A new scheme aimed at combating racial hate crime in Belfast was launched by police and migrant communities on Tuesday.
The Advocacy Scheme will see the appointment of two bilingual advocates recruited from within ethnic minority communities to work with Hate Crime, Minority Liaison and neighbourhood officers in the PSNI in the south and east Belfast.
The scheme has been in development since last year.
© Press Association