"I'm not doing deals with the Scottish National Party... it's not happening. I'm working for a majority Labour government," Miliband said in a BBC interview.
Miliband leads the centre-left Labour party which is virtually neck and neck in opinion polls with Prime Minister David Cameron's centre-right Conservatives before May 7's vote.
This indicates that neither of the two main parties will win outright and will have to team up with one or more smaller parties to form a coalition or minority government.
Miliband's comments come as the Conservatives, facing accusations they have fought a negative and insufficiently passionate campaign, increasingly emphasise what they say are the dangers of an alliance between Labour and the SNP.
Cameron's party claims the SNP would pull Labour further to the left and put the United Kingdom at risk by pushing for another referendum. They are running a high-profile poster campaign depicting Miliband as Sturgeon's puppet.
With the Conservatives increasing their focus on the Scottish issue, Miliband appeared to rule out a "confidence and supply" agreement with the SNP during his BBC interview.
This is a deal in which a smaller party supports a minority government in House of Commons confidence motions and votes on government spending.
The Labour leader has already said he would not enter a formal coalition with the SNP, much of whose support is coming from former Labour voters.
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